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  • The Compensation Effect Mechanism of Fe–Ni Mixed Prussian Blue Analogues in Aqueous Rechargeable Aluminum‐Ion Batteries
    ChemSusChem (IF 7.804) Pub Date : 2020-01-27
    Yaning Gao; Haoyi Yang; Xinran Wang; Ying Bai; Na Zhu; Shuainan Guo; Liumin Suo; Hong Li; Huajie Xu; Chuan Wu
    更新日期:2020-01-27
  • Solvent Effects on Degradative Condensation Side Reactions of Fructose in Its Initial Conversion to 5‐Hydroxymethylfurfural
    ChemSusChem (IF 7.804) Pub Date : 2020-01-27
    Xing Fu; Yexin Hu; Yanru Zhang; Yucheng Zhang; Dianyong Tang; Liangfang Zhu; Changwei Hu
    更新日期:2020-01-27
  • Side‐view Operando Optical Microscopy Analysis of a Graphite Anode to Study Its Kinetic Hysteresis
    ChemSusChem (IF 7.804) Pub Date : 2020-01-27
    Sujin Kang; Su Jeong Yeom; Hyun-Wook Lee

    Operando analyses have provided several breakthroughs in the construction of high‐performance materials and devices, including energy storage systems. However, despite the advances in electrode engineering, the formidable issues of lithium intercalation and deintercalation kinetics cannot be investigated via planar observations. Thus, we propose the side‐view operando observation by optical microscopy of a graphite anode based on its color changes during electrochemical lithiation. Since the graphite color varies according to the optical energy gap during lithiation and delithiation, we could study the corresponding charge/discharge kinetics; in addition, our cell configuration uses liquid electrolytes similarly to commercial cells, allowing practical applications. Furthermore, this side‐view observation has showed that microscale spatial variations in rate and composition control the insertion and desertion, revealing the kinetics through the whole electrode. The results of this study could enhance the fundamental understanding of the kinetics of battery materials.

    更新日期:2020-01-27
  • Assessing the viability of recovering hydroxycinnamic acids from lignocellulosic biorefinery alkaline pretreatment waste streams
    ChemSusChem (IF 7.804) Pub Date : 2020-01-26
    Steven D Karlen; Peyman Fasahati; Mona Mazaheri; Jose Serate; Rebecca A Smith; Sirisha Sirobhushanam; Mingjie Chen; Vitaliy I Tymkhin; Cynthia L Cass; Sarah Liu; Dharshana Padmakshan; Dan Xie; Yaoping Zhang; Mick A McGee; Jason D Russell; Joshua J Coon; Heidi F Kaeppler; Natalia de Leon; Christos T Maravelias; Troy M Runge; Shawn M Kaeppler; John C Sedbrook; John Ralph

    The hydroxycinnamic acids, p ‐coumaric acid ( p CA) and ferulic acid (FA), add diversity to the portfolio of products produced by grass‐fed lignocellulosic biorefineries. The level of lignin‐bound p CA in Zea mays was modified by alteration of PMT expression. The biomass was processed in a lab‐scale alkaline‐pretreatment biorefinery process and the data was used for a baseline technoeconomic analysis to determine where to direct our future research efforts in coupling plant design to biomass utilization processes. We concluded that future plant engineering efforts should focus on strategies that ramp up predominantly one type of hydroxycinnamate ( p CA or FA) and suppress accumulation of the other. The technoeconomic analysis indicated that target extraction titers of one hydroxycinnamic acid need to be >50 g/kg biomass, at least a five‐fold higher than our observed titers for the impure p CA/FA product mixture from wild‐type maize. The technical challenge for process engineers is to develop a viable process requiring more than 80% reduction in the isolation costs.

    更新日期:2020-01-27
  • Eutectic synthesis of high entropy metal phosphide for electrocatalytic water splitting
    ChemSusChem (IF 7.804) Pub Date : 2020-01-25
    Tiancheng Mu; Xinhui Zhao; Zhimin Xue; Wenjun Chen; Yaqing Wang

    High entropy materials, a new class of alloys that incorporate five or more principal elements into single‐phase crystal structures, have received attractive interests in materials science and engineering. Considering the tailored composition and disordered configuration, these high entropy materials may arouse functional synergism towards electrocatalysis. Here, a new strategy for preparing high‐entropy metal phosphide (HEMP) is proposed via eutectic solvent method. The as‐prepared HEMP possesses a single metal phosphide phase with up to five homogenously distributed metal components. The versatile application of high entropy materials is highlighted by integrating HEMP catalyst into a two‐electrode configuration for electrocatalytic water splitting.

    更新日期:2020-01-26
  • Hydrothermal Liquefaction of α‐O‐4 Aryl‐Ether Linkages in Lignin
    ChemSusChem (IF 7.804) Pub Date : 2020-01-24
    Matthew Yuk-Yu Lui; Bun Chan; Alexander Kah Liem Yuen; Anthony Masters; Thomas Maschmeyer

    Using lignin model compounds with relevant key characteristic structural features, the reaction pathways of α ‑O‑4 aryl‐ether linkages under hydrothermal conditions were elucidated. Our experimental results and computational modelling suggest that the α ‑O‑4 linkages in lignin undergo catalyzed hydrolyses and eliminations to give phenolic and alkenylbenzene derivatives as major products in subcritical water. The decreased relative permittivity of water at these high temperatures and pressures facilitates the elimination reactions. The alkyl group on the α ‐carbon and the methoxy groups on the phenyl rings both have positive effects on the rate of conversion of α ‑O‑4 linkages in native lignin.

    更新日期:2020-01-24
  • Cross‐linking Effects on Performance Metrics of Phenazine‐Based Polymer Cathodes
    ChemSusChem (IF 7.804) Pub Date : 2020-01-23
    Cara N. Gannett; Brian M. Peterson; Luxi Shen; Jeesoo Seok; Brett P. Fors; Héctor Abruña

    Developing cathodes that can support high charge‐discharge rates would improve the power density of lithium ion batteries. Herein, we report the development of high power cathodes, without sacrificing energy density. N,N ’‐Diphenyl phenazine was identified as a promising charge storage center by electrochemical studies due to its reversible, fast electron transfer at high potentials. By incorporating the phenazine redox units in a cross‐linked network, a high capacity (223 mAh/g), high voltage (3.45 V vs Li/Li + ) cathode material was achieved. Optimized cross‐linked materials are able to deliver reversible capacities as high as 220 mAh g –1 at 120 C with minimal degradation over 1000 cycles. The work presented here highlights the fast ionic transport and rate capabilities of amorphous, organic materials and demonstrates their potential as high energy and power density materials for next generation electrical energy storage technologies.

    更新日期:2020-01-24
  • Utilizing Cyclic Voltammetry to Understand the Energy Storage Mechanisms for Copper Oxide and its Graphene Oxide Hybrids as Lithium‐Ion Battery Anodes
    ChemSusChem (IF 7.804) Pub Date : 2020-01-23
    Cameron Day; Katie Greig; Alexander Massey; Jennifer Peake; David Crossley; Robert A. W. Dryfe
    更新日期:2020-01-23
  • An Efficient and Practical System for the Synthesis of N,N‐Dimethylformamide by CO2 Hydrogenation using a Ru‐based Heterogeneous Catalyst: From Batch to Continuous Flow
    ChemSusChem (IF 7.804) Pub Date : 2020-01-23
    Gunniya Hariyanandam Gunasekar; Sudakar Padmanaban; Kwangho Park; Kwang-Deog Jung; Sungho Yoon

    In the context of CO 2 utilization, a number of CO 2 conversion methods have been identified in laboratory‐scale research; however, only a very few transformations have been successfully scaled up and implemented industrially. The main bottleneck in realizing industrial application of these CO 2 conversions is the lack of industrially viable catalytic systems and the need of practically implementable process developments. Herein, we developed a simple, highly efficient and recyclable ruthenium‐grafted bisphosphine‐based porous organic polymer (Ru@PP‐POP) catalyst for the hydrogenation of CO 2 to N,N‐dimethylformamide, and obtained best ever turnover number (TON) of 160,000 and initial turnover frequency (TOF) of 29,000 h ‐1 in a batch process. The catalyst was successfully applied in a trickle bed reactor and utilized in an industrially feasible continuous‐flow process for the first time with an excellent durability and productivity of 915 mmol h ‐1 g Ru ‐1 .

    更新日期:2020-01-23
  • Grain enlargement and defect passivation with melamine additive for high efficiency and stable CsPbBr3 perovskite solar cells
    ChemSusChem (IF 7.804) Pub Date : 2020-01-23
    Jingwei Zhu; Benlin He; Zekun Gong; Yang Ding; Wenyu Zhang; Xueke Li; Zhihao Zong; Haiyan Chen; Qunwei Tang

    The preparation of high‐quality perovskite films with low grain boundaries and defect states is a prerequisite for achieving high‐efficiency perovskite solar cells (PSCs) with good environmental stability. In this work, an effective additive engineering for simultaneous defect passivation and crystal growth of CsPbBr3 perovskite films by introducing 1,3,5‐Triazine‐2,4,6‐triamine (melamine) into PbBr2 precursor solution is reported. Arising from the positive effect of the formed melamine‐PbBr2 film with loose large‐grained structure and decreased crystallinity on the crystallization process of perovskite, the retardation of perovskite crystallization rate caused by the interaction between melamine and lead ions and the passivation of melamine, the high‐quality CsPbBr3 perovskite film with lower grain boundaries as well as defect densities and better energy level matching is fabricated by multi‐step liquid phase spin‐coating technology, which greatly suppresses the non‐radiative recombination resulted from the defects and promotes the charge extraction at the interface. A champion power conversion efficiency as high as 9.65% with an attractive open‐circuit voltage of 1.584 V is achieved for PSCs with an architecture of FTO/c‐TiO2/m‐TiO2/melamine‐added CsPbBr3/carbon free of hole‐transporting layers. Furthermore, the encapsulated‐free melamine‐added CsPbBr3 PSC shows a superior thermal and humidity stability in ambient air with 85°C or 85% RH over 720 h.

    更新日期:2020-01-23
  • Metal‐Free, Solid‐State, Paperlike Rechargeable Batteries Consisting of Redox‐Active Polyethers
    ChemSusChem (IF 7.804) Pub Date : 2020-01-22
    Kan Hatakeyama‐Sato; Toshiki Tezuka; Rieka Ichinoi; Satoshi Matsumono; Karin Sadakuni; Kenichi Oyaizu
    更新日期:2020-01-23
  • Catalytic Production of Glucose–Galactose Syrup from Greek Yogurt Acid Whey in a Continuous‐Flow Reactor
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Mark J. Lindsay; Kefeng Huang; Brent A. Buchinger; Cristos T. Maravelias; James A. Dumesic; Scott A. Rankin; George W. Huber
    更新日期:2020-01-23
  • Gel–Emulsion‐Templated Polymeric Aerogels for Water Treatment by Organic Liquid Removal and Solar Vapor Generation
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Jianfei Liu; Hui Yang; Kaiqiang Liu; Rong Miao; Yu Fang
    更新日期:2020-01-23
  • Trapping of Polysulfides with Sulfur‐Rich Poly Ionic Liquid Cathode Materials for Ultralong‐Life Lithium–Sulfur Batteries
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Xu Liu; Yu Lu; Qinghui Zeng; Pingping Chen; Zhenfeng Li; Xin Wen; Wen Wen; Zengxi Li; Liaoyun Zhang
    更新日期:2020-01-23
  • Natural Polymers as Green Binders for High‐Loading Supercapacitor Electrodes
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Peter Ruschhaupt; Alberto Varzi; Stefano Passerini
    更新日期:2020-01-23
  • Microscopic Properties of Na and Li—A First Principle Study of Metal Battery Anode Materials
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Daniel Gaissmaier; Matthias van den Borg; Donato Fantauzzi; Timo Jacob
    更新日期:2020-01-23
  • 更新日期:2020-01-23
  • Regioselective β‐Arylation of α‐Angelica Lactone through Isomerization/Addition under Mild Conditions
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Kai‐Feng Zhuo; Shang‐Hai Yu; Tian‐Jun Gong; Yao Fu
    更新日期:2020-01-23
  • Enhanced Conversion of Xylan into Furfural using Acidic Deep Eutectic Solvents with Dual Solvent and Catalyst Behavior
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Eduarda S. Morais; Mara G. Freire; Carmen S. R. Freire; João A. P. Coutinho; Armando J. D. Silvestre
    更新日期:2020-01-23
  • Molecular Engineering of Fully Conjugated sp2 Carbon‐Linked Polymers for High‐Efficiency Photocatalytic Hydrogen Evolution
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Tao Huang; Xi Lin; Yang Liu; Jiwu Zhao; Huan Lin; Ziting Xu; Shuncong Zhong; Chunjie Zhang; Xuxu Wang; Xianzhi Fu; Jinlin Long
    更新日期:2020-01-23
  • Controllable Fabrication and Li Storage Kinetics of 1 D Spinel LiMn2O4 Positive Materials for Li‐ion Batteries: An Exploration of Critical Diameter
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Chengyi Zhu; Yannan Zhang; Xiaohua Yu; Peng Dong; Jianguo Duan; Jiaming Liu; Jianxiong Liu; Yingjie Zhang
    更新日期:2020-01-23
  • Electrolyte imbalance determination of a vanadium redox flow battery by potential‐step analysis of the initial charging
    ChemSusChem (IF 7.804) Pub Date : 2020-01-22
    Kirstin Beyer; Jan grosse Austing; Barbara Satola; Timo Di Nardo; Marco Zobel; Carsten Agert

    Vanadium redox flow batteries (VRFB) suffer from capacity fades due to side reactions and crossover effects through the membrane. These processes lead to a deviation of the optimal initial average oxidation state (AOS = +3.5) of vanadium species in both half‐cell electrolytes. In order to rebalance the electrolyte solutions, it is first necessary to determine the current AOS. In this study a new method is presented that enables a precise determination of the AOS. A potential‐step analysis is performed with mixed electrolyte solutions of both half‐cells during the initial charging. The potential is recorded with a simple OCV cell and the potential‐steps are analyzed. A correlation between the duration of the potential plateaus in the OCV and the amount of vanadium ions of a certain oxidation state in the half‐cell electrolytes was found and is used to determine the AOS precisely with a maximum error of 3.6 %.

    更新日期:2020-01-23
  • Molecular design strategy towards high‐redox‐potential and low soluble n‐type phenazine derivatives as cathode materials for lithium batteries
    ChemSusChem (IF 7.804) Pub Date : 2020-01-22
    Jun Chen; Licheng Miao; Luojia Liu; Kai Zhang

    N‐type phenazine (PZ) derivatives represent an emerging class of cathode materials in lithium batteries for low‐cost and sustainable energy storage. However, the low redox potential (< 2 V) and high solubility severely plague their application to battery systems. To explore and solve such problems in lithium batteries, we here systematically investigate the redox characteristics of 13 types of n‐type PZ derivatives and their dissolution behavior in 7 organic electrolytes using density functional theory (DFT) calculations, and then summarize their rules. Two decisive factors are observed to tune the redox potentials for these molecules: one is the electron density around N active sites, the other is the chelation on lithium by both active N and substituent group. Specific approaches including reducing aromatic rings and introducing functional groups at β sites in n‐type PZ derivatives can improve the redox potential to ~3 V. In addition, we develop a new index denoted as Ediff to investigate the solubility of n‐type PZ derivatives. The most effective way to reduce the dissolution of electrodes in solvents is accordingly proposed as to improve intermolecular attraction between electrode molecules through introducing π‐π stacking and hydrogen bonds. Such an all‐around guideline should enlighten and promote the application of n‐type PZ‐based organic cathodes with high‐redox potential and low electrode solubility for lithium batteries.

    更新日期:2020-01-23
  • Zeolite Nanocrystals Embedded in Microcellular Carbon Foam as a High‐Performance CO2 Capture Adsorbent with Energy‐Saving Regeneration Properties
    ChemSusChem (IF 7.804) Pub Date : 2020-01-22
    Sebastijan Kovacic; Matjaž Mazaj; Milan Bjelica; Ema Žagar; Nataša Zabukovec Logar; Sebastijan Kovačič

    Here, we report the facile synthesis of four‐length‐scaled hierarchically structured porous carbon nanocomposite via emulsion‐template strategy. Such previously unreported combination of zeolite nanocrystals embedded in the walls of microcellular carbon foam gives unique textural and structural properties ensuring excellent ability to selectively capture CO2 due to presence of ultramicropores. The zeolite–microcellular carbon foam synergism delivers adsorbent with significantly enhanced CO2 capture capacity of up to 5 mmol·g‐1, CO2/N2 selectivity of up to 80 and outstanding multi‐cycle capture performance under humid conditions (70% performance retention after 30 regeneration cycles). More impressively, electrically conductive carbon framework enables Joule heating and cooling capability, and thus fast and energy efficient regeneration, with an estimated energy consumption of only about 12 kWh.

    更新日期:2020-01-23
  • 更新日期:2020-01-22
  • Engineering Active Fe Sites on Nickel–Iron Layered Double Hydroxide through Component Segregation for Oxygen Evolution Reaction
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Chunlei Peng; Nian Ran; Gang Wan; Wanpeng Zhao; Zhaoyu Kuang; Zheng Lu; Chengjun Sun; Jianjun Liu; Lianzhou Wang; Hangrong Chen
    更新日期:2020-01-22
  • Recent Progress in Two‐Dimensional Layered Double Hydroxides and Their Derivatives for Supercapacitors
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Xiaorui Gao; Peikui Wang; Zhenghui Pan; Jerome P. Claverie; John Wang
    更新日期:2020-01-22
  • Value‐Added Formate Production from Selective Methanol Oxidation as Anodic Reaction to Enhance Electrochemical Hydrogen Cogeneration
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Mei Li; Xiaohui Deng; Kun Xiang; Yue Liang; Bin Zhao; Jie Hao; Jing‐Li Luo; Xian‐Zhu Fu
    更新日期:2020-01-22
  • Simple and Eco‐Friendly Fabrication of Electrode Materials and Their Performance in High‐Voltage Lithium‐Ion Batteries
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Lucía Barbosa; Fernando Luna‐Lama; Yarivith González Peña; Alvaro Caballero
    更新日期:2020-01-22
  • One‐Pot Synthesis of a Copolymer Micelle Crosslinked Binder with Multiple Lithium‐Ion Diffusion Pathways for Lithium–Sulfur Batteries
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Rongnan Guo; Shunlong Zhang; Jianli Wang; Hangjun Ying; Weiqiang Han
    更新日期:2020-01-22
  • Mechanistic Investigation of a Hybrid Zn/V2O5 Rechargeable Battery with a Binary Li+/Zn2+ Aqueous Electrolyte
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Dauren Batyrbekuly; Sabrina Cajoly; Barbara Laïk; Jean‐Pierre Pereira‐Ramos; Nicolas Emery; Zhumabay Bakenov; Rita Baddour‐Hadjean
    更新日期:2020-01-22
  • Effective Singlet Oxygen Generation in Silica‐Coated CsPbBr3 Quantum Dots through Energy Transfer for Photocatalysis
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Kailun Gu; Yu Wang; Jianhua Shen; Jingrun Zhu; Yihua Zhu; Chunzhong Li
    更新日期:2020-01-22
  • 更新日期:2020-01-22
  • Solvent Effects on Degradative Condensation Side Reactions of Fructose in Its Initial Conversion to 5‐Hydroxymethylfurfural
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Xing Fu; Yexin Hu; Yanru Zhang; Yucheng Zhang; Dianyong Tang; Liangfang Zhu; Changwei Hu
    更新日期:2020-01-22
  • Efficient Plastic Waste Recycling to Value‐Added Products by Integrated Biomass Processing
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Kassem Beydoun; Jürgen Klankermayer
    更新日期:2020-01-22
  • Metal‐Nitrogen‐Carbon Electrocatalysts for CO2 Reduction Towards Syngas Generation
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Laurent Delafontaine; Tristan Asset; Plamen Atanassov

    Shifting syngas (a H 2 :CO mix) production away from fossil‐fuel dependent methods ( e.g. , steam methane reforming and coal gasification) is mandatory as syngas is of interest as both a fuel and as a value‐added chemical precursor. When using the adequate electrocatalysts, such as silver‐based or metal‐nitrogen‐carbon (M‐N‐C), the electrochemical CO 2 reduction reaction (CO 2 RR) allows for the production of CO alongside H 2 (from the hydrogen evolution reaction), thus leading to syngas generation. Here, we discuss the application of M‐N‐C electrocatalysts for syngas generation. The mechanisms leading to different faradaic selectivity for CO are reviewed as a function of the metallic element nature, using both computational and experimental approaches. The role played by the metal‐free moieties in the metal‐nitrogen‐carbon electrocatalysts is underlined. Since the M‐N‐C electrocatalysts only recently entered the CO 2 RR field ( vs. the Cu, Ag or Au‐based nanostructures), they have been mainly characterized in static liquid environments, where the reaction rate is significantly hampered by CO 2 ‐dissolution/diffusion limitations. Therefore, the design of CO 2 RR electrolyzers for M‐N‐C electrocatalysts is here addressed, highlighting designs such as zero‐gap electrolyzers using anionic membranes and humidified CO 2 gas feed at the cathode.

    更新日期:2020-01-22
  • D‐band Centers Engineering of Perovskite Cobaltite for Enhanced Electrocatalytic Oxygen Evolution
    ChemSusChem (IF 7.804) Pub Date : 2020-01-21
    Yiqiang Sun; Zihan Zhao; Si Wu; Wenjuan Li; Bo Wu; Guangning Liu; Guozhu Chen; Bo Xu; Baotao Kang; Yue Li; Cuncheng Li

    Great efforts have been made to understand and upgrade the kinetically sluggish oxygen evolution reaction (OER). Herein, a series of V doped LaCoO 3 (V‐LCO) OER electrocatalysts with optimized d band center are successfully fabricated. When utilized as electrode for the OER, as‐formed V‐LCO‐II demands overpotential of only 306 mV to drive a geometrical catalytic current density of 10 mA cm ‐2 . Furthermore, at a given overpotential of 350 mV, the OER current density of V‐LCO‐II is about 22 times that of pure LCO nanoparticles. The V dopant tailored d‐band center facilitate the adsorption of OER intermediates, and promote the formation of amorphous active species on the surface of LCO due to the notable exchange interaction between high‐spin V 4 + and low‐spin Co 2+ . This work may create new opportunities for developing other high active OER catalysts via d band centers engineering.

    更新日期:2020-01-22
  • Construction of Defective Zinc–Cadmium–Sulfur Nanorods for Visible‐Light‐Driven Hydrogen Evolution Without the Use of Sacrificial Agents or Cocatalysts
    ChemSusChem (IF 7.804) Pub Date : 2020-01-20
    Guoqiang Zhang; Xiang Ling; Guoshuai Liu; Yangsen Xu; Shuning Xiao; Qitao Zhang; Xun Yang; Chuntian Qiu; Hongwei Mi; Chenliang Su
    更新日期:2020-01-21
  • A Composite Bifunctional Oxygen Electrocatalyst for High‐Performance Rechargeable Zinc–Air Batteries
    ChemSusChem (IF 7.804) Pub Date : 2020-01-20
    Jia‐Ning Liu; Bo‐Quan Li; Chang‐Xin Zhao; Jia Yu; Qiang Zhang
    更新日期:2020-01-21
  • Thermal Cracking of Sugars for the Production of Glycolaldehyde and Other Small Oxygenates
    ChemSusChem (IF 7.804) Pub Date : 2020-01-20
    Christian B. Schandel; Martin Høj; Christian M. Osmundsen; Anker D. Jensen; Esben Taarning
    更新日期:2020-01-21
  • Anodically Triggered Aldehyde Cation Auto‐Catalysis for Alkylation of Heteroarenes
    ChemSusChem (IF 7.804) Pub Date : 2020-01-20
    Kedong Yuan; Caiyan Liu; Zihui Xiao; Shuhua Wu; Yongli Shen; Yi Ding

    Alkylation of heteroarenes using aldehydes is a direct approach to increase molecular complexity, which however often involves the usage of stochiometric oxidant, strong acid and high temperature. Herein, we report an energy‐efficient electrochemical alkylation of heteroarenes using aldehydes under mild conditions without mediators. Interestingly, the graphite anode can trigger aldehyde cationic species, which act as the effective auto‐catalysts to react with a range of heteroarene to produce the corresponding products with excellent regioselectivity and in high yields. Compared to the traditional electro‐synthesis approaches, this electro‐triggered reaction provides an electricity‐saving and eco‐friendly route to high value chemicals.

    更新日期:2020-01-21
  • A Metal‐free Donor‐Acceptor Covalent Organic Framework Photocatalyst for Visible‐Light‐Driven Reduction of CO2 with H2O
    ChemSusChem (IF 7.804) Pub Date : 2020-01-20
    Kai Lei; Di Wang; Mingpu Kou; Zhaoyu Ma; Li Wang; Liqun Ye; Yan Kong

    Visible‐light‐driven CO 2 reduction to valuable chemicals without sacrificial agents and co‐catalysts remains challenging, especially for metal‐free photocatalytic systems. Herein, we report a novel donor‐acceptor (D‐A) COF (CT‐COF) that was constructed by the Schiff base reaction of carbazole‐triazine based D‐A monomers and possessed a suitable energy band structure, strong visible‐light‐harvesting and rich nitrogen sites. CT‐COF used as a metal‐free photocatalyst can reduce CO 2 with gaseous H 2 O to CO as the main carbonaceous product with the approximate stoichiometric O 2 evolution under visible light irradiation and co‐catalysts free conditions. The CO evolution rate (102.7 μmol g ‐1 h ‐1 ) is 68.5 times that of g‐C 3 N 4 under the same test conditions. In situ FT‐IR analysis indicates that CT‐COF could adsorb and activate the CO 2 and H 2 O molecules and that COOH* species may be a key intermediate. DFT calculations suggest that nitrogen atoms in the triazine rings may be photocatalytic active sites.

    更新日期:2020-01-21
  • The key for lignin solution self‐assembly: AFM force measurement and MD simulation study for dissolution and aggregation mechanisms of lignin in organic solvent‐water
    ChemSusChem (IF 7.804) Pub Date : 2020-01-17
    Jingyu Wang; Yong Qian; Libo Li; Xueqing Qiu

    Lignin‐based nanomaterials fabricated by solution self‐assembly in organic solvent‐water mixture is one of the most attractive biomass product. In order to accurately control the structure, size, and property of lignin‐based nanomaterials, it is important to achieve the fundamental understanding for its dissolution and aggregation mechanisms. In this work, atomic force microscope (AFM) and molecular dynamic (MD) simulation were employed to explore the dissolution and aggregation behavior of enzymatic hydrolysis lignin (EHL) in different organic solvent‐water mixtures at molecular scale. Results show that EHL was well dissolved in appropriate organic solvent‐water mixture, such as acetone‐water mixture with volume ratio of 7:3, while EHL aggregated in pure water, ethanol, acetone, tetrahydrofuran. The interactions between EHL‐coated AFM probe and substrate were 1.21 ± 0.18 and 0.75 ± 0.35 mN/m respectively in water and acetone. In comparison, such interaction decreased to 0.15 ± 0.08 mN/m in acetone‐water mixture. MD simulation further indicates that hydrophobic skeleton and hydrophilic groups of lignin could be solvated by acetone and water molecules respectively, which significantly promoted the dissolution of lignin. Conversely, only hydrophobic skeleton or hydrophilic group was solvated in organic solvent or water inducing serious aggregation of lignin.

    更新日期:2020-01-21
  • Promote the voltage of organic cathode materials by diluting the electron density in the π‐conjugated skeleton
    ChemSusChem (IF 7.804) Pub Date : 2020-01-17
    Gaole Dai; Yehua Gao; Zhihui Niu; Ping He; Xiaohong Zhang; Yu Zhao; Haoshen Zhou

    Organic compounds as battery materials are promising because of their resource sustainability as well as the structural tunability and potentially low‐cost. But when serving as the positive electrode, the working voltage is relatively low compared with the inorganic counterpart. Here, we demonstrate a strategy by diluting the electron density of N‐based redox center in conjugated organics to promote the discharge voltage. Compared with electron‐rich heterocyclic compounds that utilize N as the redox center, the pentatomic rings like carbazole derivatives exhibit higher atomic‐dipole‐moment‐corrected Hirshfeld (ADCH) charge population over the hexatomic ones, which leads to a significant increase in the oxidation potential. As a result, an as‐designed polymeric indolocarbazole derivative shows a high discharge voltage of 3.7–4.3 V versus Li + /Li with decent cycling performance. Such a strategy may be applicable to design high‐voltage organic electrode materials with other redox centers.

    更新日期:2020-01-21
  • Precursor‐Engineering Coupled Microwave Molten‐Salt Strategy Enhances Photocatalytic Hydrogen Evolution Performance of g‐C3N4 Nanostructures
    ChemSusChem (IF 7.804) Pub Date : 2020-01-17
    Huijuan Jing; Mingzhu You; Shasha Yi; Tao Li; Haipeng Ji; Yu Wang; Zongtao Zhang; Rui Zhang; Deliang Chen; Huaming Yang
    更新日期:2020-01-17
  • Synthesis of NH‐Sulfoximines Using Recyclable Hypervalent Iodine (III) Reagents under Aqueous Micellar Conditions
    ChemSusChem (IF 7.804) Pub Date : 2020-01-17
    Guocai Zhang; Hongsheng Tan; Weichun Chen; Hong C. Shen; Yue Lu; Changwu Zheng; Hongxi Xu

    The synthesis of NH‐sulfoximines from sulfides has been first developed under a mild, sustainable condition in an aqueous solution with surfactant TPGS‐750‐M as the catalyst at room temperature. In this newly developed process, a simple and convenient recyclable strategy to regenerate the indispensable hypervalent iodine(III) was utilized. The resulting 1,2,3‐trifluoro‐5‐iodobezene could be recovered almost quantitively from the mixture by liquid‐liquid extraction, and then oxidized to the corresponding iodine (III) species. This optimized protocol is compatible with a broad range of functional groups and could be easily performed on a gram scale. Thus, this novel method provides a new and green protocol for the synthesis of sulfoximines.

    更新日期:2020-01-17
  • Response‐Surface‐Optimized and Scaled‐Up Microbial Electrosynthesis of Chiral Alcohols
    ChemSusChem (IF 7.804) Pub Date : 2020-01-17
    Jeannine C. Mayr; Luis F. M. Rosa; Natalia Klinger; Jan-Hendrik Grosch; Falk Harnisch; Antje C. Spiess

    A whole variety of enzymes can be easily incorporated and overexpressed within Escherichia coli cells via plasmids, making it an ideal chassis for bioelectrosynthesis. We recently demonstrated microbial electrosynthesis (MES) of chiral alcohols using genetically modified E. coli with plasmid‐incorporated and overexpressed enzymes and methyl viologen as mediator for electron transfer. Here, this model system, using NADPH‐dependent alcohol dehydrogenase from Lactobacillus brevis to convert acetophenone to ( R )‐1‐phenylethanol, was assessed by a Design of Experiment (DoE) approach. Process optimization was achieved with a 2.4‐fold increased yield of 94±7%, a 3.9‐fold increased reaction rate of 324±67 μM h ‐1 , and a coulombic efficiency of up to 68±7%, while maintaining an excellent enantioselectivity of >99%. Subsequent scale‐up to 1 L using electrobioreactors under batch and fed‐batch conditions increased the titer of ( R )‐1‐phenylethanol to 12.8±2.0 mM and paves the way to further develop E. coli into a universal chassis for MES in a standard biotechnological process environment.

    更新日期:2020-01-17
  • Mild and Efficient Synthesis of Diverse Organo‐Au(I)‐L Complexes in Green Solvents
    ChemSusChem (IF 7.804) Pub Date : 2020-01-17
    Fredric J. L. Ingner; Ann-Cathrin Schmitt; Andreas Orthaber; Paul J. Gates; Lukasz T Pilarski

    An exceptionally mild and efficient method is presented for the preparation of (hetero)aryl‐Au I ‐L complexes using ethanol or water as the reaction medium at room temperature and R‐B(triol)K boronates as the transmetalation partner. The reaction returns up to quantitative yields, needs no exogeneous base or other additives and a simple filtration is the only required purification method, which obviates considerable waste associated with alternative workup methods. A broad reaction scope is demonstrated with respect to both the L and (hetero)aryl ligands on product Au complexes. Despite the polar reaction medium, large polycyclic aromatic hydrocarbon units can be incorporated on the product Au complexes in very good to excellent yields. We demonstrate the use of our approach for the chemoselective manipulation of orthogonally protected aryl boronates to afford a novel new class of NHC‐Au‐aryl complexes. A mechanistic rationale is proposed.

    更新日期:2020-01-17
  • Solution‐processable thermally crosslinked organic radical polymer battery cathodes
    ChemSusChem (IF 7.804) Pub Date : 2020-01-17
    Jodie Lutkenhaus; Shaoyang Wang; Albert Min Gyu Park; Ting Ma; Fei Li; Alexandra Easley; Gregory D. Fuchs

    Due to rapid charge transfer and high cycling stability, organic radical polymers have been viewed as a promising cathode material for next‐generation batteries. However, these organic polymer electrodes gradually dissolve in the electrolyte, resulting in capacity fade. Previous literature has reported several crosslinking methods, but they are either not compatible with carbon additives or compromise solution processability of the electrodes. Here, we present a one‐step post‐synthetic, carbon‐compatible crosslinking method that effectively crosslinks the organic polymer electrode while allowing for easy solution processing. The highest electrode capacity of 104 mAh/g (vs. theoretical capacity of 111 mAh/g) is achieved by introducing 1 mol% of the crosslinker, where as the highest capacity retention (99.6%) was obtained for 3 mol% crosslinker. In addition, we observe mass transfer in‐situ using electrochemical quartz crystal microbalance with dissipation monitoring (QCM‐D). Our results may guide future electrode design toward fast‐charging, high capacity organic electrodes.

    更新日期:2020-01-17
  • Direct catalytic conversion of furfural to furan‐derived amines in the presence of Ru based catalyst
    ChemSusChem (IF 7.804) Pub Date : 2020-01-16
    Shi Jiang; Wahiba Ramdani; Changru Ma; Eric Muller; Marc PERA-TITUS; François Jérôme; Karine De Oliveira Vigier

    The production of amine intermediates from biomass is capturing increasing attention. Herein we report simple and efficient preparation of l furan‐derived amines (for instance 1‐(furan‐2‐yl)‐4‐methylpentan‐2‐amine) with high yield (up to 95%) from ( E )‐1‐(furan‐2‐yl)‐5‐methylhex‐1‐en‐3‐one. The catalyst used was Ru/C and it was recyclable up to 4th cycle. To further realize cost‐efficiency, one‐reactor tandem concept was attempted. To this aim direct reaction from furfural was investigated. A high yield (74%) towards 1‐(furan‐2‐yl)‐4‐methylpentan‐2‐amine could be achieved starting directly from furfural in the presence of methylisobutyl ketone, NH 3 , H 2 and Ru/C catalyst.

    更新日期:2020-01-16
  • Heterogeneous rhenium oxide modified iridium catalyzed one‐pot conversion of lignin into naphthenes
    ChemSusChem (IF 7.804) Pub Date : 2020-01-16
    Changzhi Li; Bo Zhang; Xinxin Li; Xiaoli Pan; Jianwei Ji; Yujing Ren; Hua Wang; Na Ji; Qiying Liu

    Direct transformation of lignin into fuels and chemicals remains huge challenge due to the stubborn and complicated structure of lignin. Here rhenium oxide modified iridium supported by SiO 2 (Ir‐ReO x /SiO 2 ) was employed for one‐pot conversion of various lignin model compounds and lignin feedstocks into naphthenes. Up to 100% yield of cyclohexane from model compounds and 44.3% yield of naphthenes from lignin feedstocks were achieved. 2D HSQC NMR analysis before and after reaction confirmed the clear activity of Ir‐ReO x /SiO 2 in cleavage of the C‐O bonds and hydrodeoxygenation of the depolymerized products. H 2 ‐temperature‐programed reduction (H 2 ‐TPR), temperature‐programmed desorption of NH 3 (NH 3 ‐TPD), IR spectroscopy of pyridine adsorption (pyridine‐IR), X‐ray photoelectron spectroscopy (XPS) and X‐ray absorption fine structure (XAFS) characterization and control experiments revealed that a synergistic effect between Ir and ReO x in Ir‐ReO x /SiO 2 play a crucial role for the high performance, of which, ReO x was mainly responsible for the cleavage of C‐O bonds whilst Ir was in charge of HDO reaction and saruration of the benzene rings. This methodology opens an energy‐efficient route for directly converting lignin into valuable naphthenes.

    更新日期:2020-01-16
  • Biomimetic Design of 3D Transition Metal/Carbon Dyad for One‐Step Hydrodeoxygenation of Vanillin
    ChemSusChem (IF 7.804) Pub Date : 2020-01-16
    Tian-Jian Zhao; Jun-Jun Zhang; Hong-Hui Wang; Juan Su; Xin-Hao Li; Jie-Sheng Chen

    Enzyme catalysts always show the excellent catalytic selectivity, which is important in biochemistry, especially in catalytic synthesis and biopharming. This selectivity is achieved by combining the binding effect induced by the electrostatic effect of the enzyme to attract specific substrate and then pre‐arranging the substrates inside the enzyme’s pocket. Herein, we report a proof‐of‐concept application of an interfacial electrostatic field induced via constructing Schottky heterojunctions to mimic the electrostatic catalysis of enzyme. In combination with 3D structure, a transition metal/carbon dyad was designed via a nanoconfinement methods to successfully promote the differential binding effect and the space‐induced organization of reaction intermediate (vanillyl alcohol) and improved a novel one‐step hydrogenolysis route of vanillin for the production of 2‐methoxy‐4‐methylphenol with remarkably high selectivity (> 99%).

    更新日期:2020-01-16
  • Visible Light‐directly Triggered Quantitative Oxidation of 9,10‐dihydroanthracene to Anthraquinone by Molecular Oxygen under Normal Temperature and Pressure
    ChemSusChem (IF 7.804) Pub Date : 2020-01-16
    Dabo Jiang; Wenwei Hu; Mengke Chen; Zaihui Fu; Anqun Su; Bo Yang; Feng Mao; Chao Zhang; Yachun Liu; Dulin Yin

    The development of mild and efficient process for the selective oxygenation of organic compounds by molecular oxygen (O 2 ) can be one of the key technologies for synthesizing oxygenates. This paper discloses an atom‐efficient synthesis protocol for the photo‐oxygenation of 9,10‐dihydroanthracene (DHA) by O 2 to anthraquinone (AQ), which can achieve quantitative AQ yield (100%) without any extra catalysts and additives under normal temperature and pressure. Also, 86.4% AQ yield is obtained even in air atmosphere. Furthermore, this protocol has a good compatibility for the photo‐oxidation of several other compounds with a similar structure to DHA. Based on a series of control experiments and free radical quenching and EPR spin trapping results. The photo‐oxygenation of DHA is likely initiated by its photo‐excited state DHA* and the latter can activate O 2 to a superoxide anion radical (O 2 ⚫‐ ) via a transfer of its electron. Subsequently, this photo‐oxidation is gradually dominated by the oxygenated product AQ as an active photo‐catalyst, obtained from the oxidation of DHA by O 2 ⚫‐ , and it is accelerated with the rapid accumulation of AQ. The present photo‐oxidation protocol gives a good example for the selective oxygenation based on the photo‐excited substrate self‐activated O 2 , which compliances well with ‘green’ chemistry ideals.

    更新日期:2020-01-16
  • Improving artificial photosynthesis in carbon nitride by gas‐liquid‐solid Interface management for full light‐induced CO2 reduction to C1‐C2 fuels and O2
    ChemSusChem (IF 7.804) Pub Date : 2020-01-15
    Yang Xia; Kai Xiao; Bei Cheng; Jiaguo Yu; Lei Jiang; Markus Antonietti; Shaowen Cao

    The activity and selectivity of simple photocatalysts for CO2 reduction were still limited by the insufficient photophysics of the catalysts, but also the low solubility and slow mass transport of gas molecules in/through aqueous solution. Herein, we present a way to overcome these limitation by constructing a triphase photocatalytic system, in which polymeric carbon nitride (CN) is immobilized onto a hydrophobic substrate, and the photocatalytic reduction reaction occurs at a gas‐liquid‐solid (CO2‐water‐catalyst) triple connection. It is found that the CN anchored onto the surface of a hydrophobic substrate exhibits an about 7.2‐fold enhancement in the total CO2 conversion, with a rate of 415.50 μmol m‐2 h‐1 under simulated solar light irradiation. This value corresponds to an overall photosynthetic efficiency for full water‐CO2 conversion of 0.33%, i.e. very close to biological systems. Meanwhile, a remarkable enhancement of direct C2 hydrocarbon production, as well as a high CO2 conversion selectivity of 97.7% was observed. Going from water oxidation to phosphate oxidation, the quantum yield can be even increased to 1.28%.

    更新日期:2020-01-15
  • Chemoenzymatic synthesis of 5‐Hydroxymethylfurfural (HMF) derived plasticizers by coupling HMF reduction with enzymatic esterification
    ChemSusChem (IF 7.804) Pub Date : 2020-01-15
    Avelino Corma; karen sulay; JOSE MIGUEL CARCELLER; MARIA JOSE CLIMENT; SARA IBORRA

    Biobased plasticizers substitutes of phthalates have been synthetized from HMF and carboxylic acids (or esters) through a chemoenzymatic cascade process that involves as first step the reduction of 5‐hydroxymethylfurfural into 2,5‐bis(hydroxymethyl)furan (BHMF) followed by the esterification of BHMF with carboxylic acids (or esters) using a supported lipase (Novozim 435). The reduction of HMF into BHMF has been performed using monodispersed metallic Co nanoparticles with a thin carbon shell (Co@C) with high activity and selectivity. After optimization of reaction conditions (temperature, hydrogen pressure and solvent) was possible to achieve 97% conversion of HMF with 99% selectivity to BHMF after 2 h reaction time. The reduction of HMF and esterification of BHMF using carboxylic acids or vinyl esters as acyl donors by lipase have been optimized separately in batch and in fixed bed continuous reactors. The coupling of two flow reactors (for reduction and subsequent esterification) working under optimized reaction conditions allowed to obtain the diesters of BHMF in ~90 yield, while no loss of activity during 60 h of operation was observed.

    更新日期:2020-01-15
  • Design C3N4 Based Hybrid Heterojunctions for Enhanced Photocatalytic Hydrogen Production Activity
    ChemSusChem (IF 7.804) Pub Date : 2020-01-15
    Fengpo Yan; Yonghua Wu; Linqin Jiang; Xiaogang Xue; Jiangquan Lv; Lingyan Lin; Yunlong Yu; Jiye Zhang; Fugui Yang; Yu Qiu

    According to our previous research, semiconductors and metals can form an Ohmic contact with an electric field pointing to the metal, or a Schottky contact with an electric field pointing to the semiconductor. If these two types of heterojunctions were constructed on a single nanoparticle, then the two electric fields may bring a synergistic effect and increase the separation rate of the photogenerated electron‐holes. Metal Ni and Ag nanoparticles were successively loaded on the g‐C 3 N 4 surface by the precipitation method and the photoreduction method in the hope of forming hybrid heterojunctions on a single nanoparticls. TEM/HRTEM images show that Ag and Ni are loaded on different locations on C3N4, which indicates that during the photoreduction reaction, Ag + obtain electrons from C 3 N 4 in the reduction reaction, while oxidation reactions are proceeded on Ni nanoparticles. Photocatalytic hydrogen production experiments show that C 3 N 4 based hybrid heterojunctions can greatly improve the photocatalytic activity of materials. The possible reason is that two heterojunctions can form a long‐range electric field similar to the p‐i‐n structure in semiconductor. Most of the photo‐generated carriers are generated and then separated in this electric field, thereby increasing the separation rate of electrons and holes. This further improves the photocatalytic activity of C 3 N 4 .

    更新日期:2020-01-15
  • Preparative‐Scale Enzymatic Synthesis of rac‐Glycerol‐1‐phosphate from Crude Glycerol Using Acid Phosphatases and Phosphate
    ChemSusChem (IF 7.804) Pub Date : 2020-01-15
    Gábor Tasnádi; Marcin Staśko; Klaus Ditrich; Mélanie Hall; Kurt Faber

    Biodiesel production automatically yields large amounts of glycerol as by‐product, which lately has raised interest toward its valorization. In addition to its use as an energy source directly, the chemical modification of glycerol may also result in value‐added derivatives. Herein, acid phosphatases employed in the synthesis mode were evaluated for the enzymatic phosphorylation of glycerol. Non‐specific acid phosphatases could tolerate glycerol concentrations up to 80 wt% and pyrophosphate concentrations up to 20 wt%, leading to product titers up to 167 g L ‐1 in a kinetic approach. In the complementary thermodynamic approach, phytases were able to directly condense glycerol and inorganic monophosphate. This unexpected behavior enabled simple and cost‐effective production of rac‐glycerol‐1‐phosphate from crude glycerol obtained from a biodiesel plant. A preparative‐scale synthesis at 100 mL‐scale resulted in the production of 16.6 g rac‐glycerol‐1‐phosphate with reasonable purity (~75%).

    更新日期:2020-01-15
  • Gelless Secondary Growth of Zeolitic Aluminophosphate SAPO‐34 and AlPO‐18 Membranes on Various Porous Support Configurations with High Performance in CO2/CH4 Separation
    ChemSusChem (IF 7.804) Pub Date : 2020-01-13
    Quang Thanh Le; Duy Hoai-Phuong Nguyen; Nha Minh Nguyen; Duy Phuc-Hoang Nguyen; Tung Ngoc Nguyen; Tung Cao-Thanh Pham

    Zeolitic Aluminophosphate, a three dimensional microporous material with the pore size of 0.38 nm is good candidate for molecular sieve application in CO 2 gas separation. The separation of CO 2 /CH 4 gas mixture is necessary for precombustion process which is meaningful in both environmental and energy efficient point of views. We report here an environmental friendly method to synthesize zeolitic aluminophosphate thin films on various configurations and low cost kaolin porous substrates with the high performance in separation of CO 2 /CH 4 mixture. The membranes are prepared by gelless seed growth method with using less amount of chemicals, no liquid gel and chemical waste, no by‐product and no washing water generated. The obtained membranes show very high selectivity for CO 2 with the separation factor of CO 2 to CH 4 is above 1,000 in the separation experiment of CO 2 /CH 4 gas mixture.

    更新日期:2020-01-14
  • Recent Advances of 2D Nanomaterials for electrochemical capacitors
    ChemSusChem (IF 7.804) Pub Date : 2020-01-13
    Tingting Huang; Yuan Jiang; Guozhen Shen; Di Chen

    Two‐dimensional (2D) nanomaterials have drawn a wide range of research interests because of their unique ultrathin layered structures and attractive properties. Especially, the electrochemical properties and great variety of 2D nanomaterials make they are highly attractive candidates for electrochemical capacitors (ECs), such as supercapacitors, lithium ion capacitors and sodium ion capacitors. Herein, we provide a comprehensive review on recent progress towards the applications of 2D nanomaterials for electrochemical capacitors. Several typical types of 2D nanomaterials were first briefly introduced, followed with the detailed descriptions on their electrochemical capacitors applications. Finally, the research perspectives and the future research directions of these interesting areas are also provided.

    更新日期:2020-01-14
  • An Insoluble Anthraquinone Dimer with Near‐Plane Structure as a Cathode Material for Lithium‐Ion Batteries
    ChemSusChem (IF 7.804) Pub Date : 2020-01-10
    Jixing Yang; Hai Su; Zhuanping Wang; Pengfei Sun; Yunhua Xu
    更新日期:2020-01-13
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