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  • A spatially orthogonal hierarchically porous acid–base catalyst for cascade and antagonistic reactions
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-26
    Mark A. Isaacs; Christopher M. A. Parlett; Neil Robinson; Lee J. Durndell; Jinesh C. Manayil; Simon K. Beaumont; Shan Jiang; Nicole S. Hondow; Alexander C. Lamb; Deshetti Jampaiah; Michael L. Johns; Karen Wilson; Adam F. Lee
    更新日期:2020-10-28
  • Revealing nitrogen-containing species in commercial catalysts used for ammonia electrosynthesis
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-26
    Yifu Chen; Hengzhou Liu; Nguon Ha; Stuart Licht; Shuang Gu; Wenzhen Li
    更新日期:2020-10-28
  • Catalyst-controlled enantioselective 1,1-arylboration of unactivated olefins
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-19
    Wang Wang; Chao Ding; Guoyin Yin
    更新日期:2020-10-19
  • High-valence metals improve oxygen evolution reaction performance by modulating 3 d metal oxidation cycle energetics
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-19
    Bo Zhang; Lie Wang; Zhen Cao; Sergey M. Kozlov; F. Pelayo García de Arquer; Cao Thang Dinh; Jun Li; Ziyun Wang; Xueli Zheng; Longsheng Zhang; Yunzhou Wen; Oleksandr Voznyy; Riccardo Comin; Phil De Luna; Tom Regier; Wenli Bi; E. Ercan Alp; Chih-Wen Pao; Lirong Zheng; Yongfeng Hu; Yujin Ji; Youyong Li; Ye Zhang; Luigi Cavallo; Huisheng Peng; Edward H. Sargent
    更新日期:2020-10-19
  • Autumn round-up
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-15

    We provide herein an overview of the present issue while introducing two new features that complement our submission and publication process.

    更新日期:2020-10-16
  • Possibilities and limitations of biotechnological plastic degradation and recycling
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-12
    Ren Wei; Till Tiso; Jürgen Bertling; Kevin O’Connor; Lars M. Blank; Uwe T. Bornscheuer

    Considerable research achievements were made to address the plastic crisis using biotechnology, but this is still limited to polyesters. This Comment aims to clarify important aspects related to myths and realities about plastic biodegradation and suggests distinct strategies for a bio-based circular plastic economy in the future.

    更新日期:2020-10-12
  • Band structure engineering and defect control of Ta 3 N 5 for efficient photoelectrochemical water oxidation
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-12
    Yequan Xiao; Chao Feng; Jie Fu; Faze Wang; Changli Li; Viktoria F. Kunzelmann; Chang-Ming Jiang; Mamiko Nakabayashi; Naoya Shibata; Ian D. Sharp; Kazunari Domen; Yanbo Li

    Ta3N5 is a promising photoanode material with a theoretical maximum solar conversion efficiency of 15.9% for photoelectrochemical water splitting. However, the highest applied bias photon-to-current efficiency achieved so far is only 2.72%. To bridge the efficiency gap, effective carrier management strategies for Ta3N5 photoanodes should be developed. Here, we propose to use gradient Mg doping for

    更新日期:2020-10-12
  • Microwave-initiated catalytic deconstruction of plastic waste into hydrogen and high-value carbons
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-12
    Xiangyu Jie; Weisong Li; Daniel Slocombe; Yige Gao; Ira Banerjee; Sergio Gonzalez-Cortes; Benzhen Yao; Hamid AlMegren; Saeed Alshihri; Jonathan Dilworth; John Thomas; Tiancun Xiao; Peter Edwards

    The ubiquitous challenge of plastic waste has led to the modern descriptor plastisphere to represent the human-made plastic environment and ecosystem. Here we report a straightforward rapid method for the catalytic deconstruction of various plastic feedstocks into hydrogen and high-value carbons. We use microwaves together with abundant and inexpensive iron-based catalysts as microwave susceptors to

    更新日期:2020-10-12
  • Catalytic upcycling of high-density polyethylene via a processive mechanism
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-12
    Akalanka Tennakoon; Xun Wu; Alexander L. Paterson; Smita Patnaik; Yuchen Pei; Anne M. LaPointe; Salai C. Ammal; Ryan A. Hackler; Andreas Heyden; Igor I. Slowing; Geoffrey W. Coates; Massimiliano Delferro; Baron Peters; Wenyu Huang; Aaron D. Sadow; Frédéric A. Perras

    The overconsumption of single-use plastics is creating a global waste catastrophe, with widespread environmental, economic and health-related consequences. Here we show that the benefits of processive enzyme-catalysed conversions of biomacromolecules can be leveraged to affect the selective hydrogenolysis of high-density polyethylene into a narrow distribution of diesel and lubricant-range alkanes

    更新日期:2020-10-12
  • Chiral paddle-wheel diruthenium complexes for asymmetric catalysis
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-05
    Taku Miyazawa; Takuro Suzuki; Yuhei Kumagai; Koji Takizawa; Takashi Kikuchi; Shunsuke Kato; Akira Onoda; Takashi Hayashi; Yuji Kamei; Futa Kamiyama; Masahiro Anada; Masahiro Kojima; Tatsuhiko Yoshino; Shigeki Matsunaga

    The development of robust and reactive chiral catalysts is a fundamental aim in asymmetric catalysis, and crucial for providing efficient methods for synthesizing chiral molecules. Chiral paddle-wheel bimetallic complexes provide a highly tunable chiral environment in rhodium-catalysed asymmetric carbene/nitrene transfer reactions and Lewis acid-catalysed reactions. Chiral paddle-wheel complexes having

    更新日期:2020-10-05
  • Acidity of surface-infiltrated binary oxides as a sensitive descriptor of oxygen exchange kinetics in mixed conducting oxides
    Nat. Catal. (IF 30.471) Pub Date : 2020-10-05
    Clement Nicollet; Cigdem Toparli; George F. Harrington; Thomas Defferriere; Bilge Yildiz; Harry L. Tuller

    Improving the kinetics of O2 reduction on oxide surfaces is critical in many energy and fuel conversion technologies. Here we show that the acidity scale for binary oxides is a powerful descriptor for tuning and predicting oxygen surface exchange kinetics on mixed conducting oxides. By infiltrating a selection of binary oxides from strongly basic (Li2O) to strongly acidic (SiO2) onto the surface of

    更新日期:2020-10-05
  • Formation of thioesters by dehydrogenative coupling of thiols and alcohols with H 2 evolution
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-28
    Jie Luo; Michael Rauch; Liat Avram; Yael Diskin-Posner; Guy Shmul; Yehoshoa Ben-David; David Milstein

    Thioesters play important roles in chemistry and biology, but their synthesis generally exhibits a poor atom economy and generates copious waste. We report here the dehydrogenative coupling of alcohols and thiols to yield thioesters and evolve H2. This waste-free reaction is catalysed by an acridine-based ruthenium pincer complex in hexamethyldisiloxane as the optimal solvent without any additives

    更新日期:2020-09-28
  • Towards molecular understanding of local chemical environment effects in electro- and photocatalytic CO 2 reduction
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-28
    Andreas Wagner; Constantin D. Sahm; Erwin Reisner

    Substantial progress has recently been made in the general understanding of the interfacial CO2 reduction reaction (CO2RR) in electro- and photocatalysis, but the influence of the local chemical environment and its effects on the catalytic interface at the molecular level remains largely elusive. Here, we introduce a classification scheme to group different aspects influencing the interfacial CO2RR

    更新日期:2020-09-28
  • Tracking the formation, fate and consequence for catalytic activity of Pt single sites on CeO 2
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-21
    Florian Maurer; Jelena Jelic; Junjun Wang; Andreas Gänzler; Paolo Dolcet; Christof Wöll; Yuemin Wang; Felix Studt; Maria Casapu; Jan-Dierk Grunwaldt

    Platinum single sites are highly attractive due to their high atom economy and can be generated on CeO2 by an oxidative high-temperature treatment. However, their location and activity are strongly debated. Furthermore, reaction-driven structural dynamics have not been addressed so far. In this study, we were able to evidence platinum-induced CeO2 surface restructuring, locate platinum single sites

    更新日期:2020-09-21
  • Superelectrophilic aluminium( iii )–ion pairs promote a distinct reaction path for carbonyl–olefin ring-closing metathesis
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-21
    Ashlee J. Davis; Rebecca B. Watson; Daniel J. Nasrallah; Jessica L. Gomez-Lopez; Corinna S. Schindler

    Catalytic carbonyl–olefin metathesis reactions represent powerful synthetic strategies for alkene formation. Successful approaches for carbonyl–olefin ring-closing, ring-opening and cross metathesis have been developed in recent years, but current limitations hamper the generality of these transformations. Stronger, more efficient catalytic systems are needed to further broaden the scope of these transformations

    更新日期:2020-09-21
  • Nanometre-scale spectroscopic visualization of catalytic sites during a hydrogenation reaction on a Pd/Au bimetallic catalyst
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-21
    Hao Yin; Li-Qing Zheng; Wei Fang; Yin-Hung Lai; Nikolaus Porenta; Guillaume Goubert; Hua Zhang; Hai-Sheng Su; Bin Ren; Jeremy O. Richardson; Jian-Feng Li; Renato Zenobi

    Understanding the mechanism of catalytic hydrogenation at the local environment requires chemical and topographic information involving catalytic sites, active hydrogen species, and their spatial distribution. Here we used tip-enhanced Raman spectroscopy (TERS) to study the catalytic hydrogenation of chloronitrobenzenethiol on a well-defined Pd(submonolayer)/Au(111) bimetallic catalyst (\(p_{\rm{H}_{2}}\) = 1

    更新日期:2020-09-21
  • How to improve the lifetime of an electrocatalyst
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-16
    Alessandro Minguzzi

    The activity and the stability of an electrocatalyst are equally important, but the reasons behind deactivation processes still remain unresolved. Achieving a deeper understanding of the process will help to inhibit deactivation and improve revivification protocols.

    更新日期:2020-09-16
  • Current state and future perspectives of engineered and artificial peroxygenases for the oxyfunctionalization of organic molecules
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-16
    Marie-Cathérine Sigmund; Gerrit J. Poelarends

    Peroxygenases are attractive biocatalysts for the selective introduction of oxygen into organic molecules under mild conditions with hydrogen peroxide as the oxygen source. In addition to the identification of primary peroxygenases, different classes of enzymes were shown to display promiscuous peroxygenase activity. Even though enzymes with peroxygenase activity are promising industrial biocatalysts

    更新日期:2020-09-16
  • Main element chemistry enables gas-cylinder-free hydroformylations
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-14
    Samuel K. Pedersen; Haraldur G. Gudmundsson; Dennis U. Nielsen; Bjarke S. Donslund; Hans Christian D. Hammershøj; Kim Daasbjerg; Troels Skrydstrup

    Industrially, aldehydes are produced annually on a multimillion-tonne scale via the hydroformylation of olefins with syngas (CO/H2 mixture). Nonetheless, this transformation has not found frequent use in the laboratory. Here we report on a simple strategy for the concerted generation of syngas from two accessible and crystalline main element compounds with just water as the primary activator for syngas

    更新日期:2020-09-14
  • Self-activation of copper electrodes during CO electro-oxidation in alkaline electrolyte
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-07
    Andrea Auer; Mie Andersen; Eva-Maria Wernig; Nicolas G. Hörmann; Nico Buller; Karsten Reuter; Julia Kunze-Liebhäuser

    The development of low-temperature fuel cells for clean energy production is an appealing alternative to fossil-fuel technologies. CO is a key intermediate in the electro-oxidation of energy carrying fuels and, due to its strong interaction with state-of-the-art Pt electrodes, it is known to act as a poison. Here we demonstrate the ability of Earth-abundant Cu to electro-oxidize CO efficiently in alkaline

    更新日期:2020-09-08
  • Catalytic-state structure and engineering of Streptococcus thermophilus Cas9
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-07
    Yifei Zhang; Hongyuan Zhang; Xuexia Xu; Yujue Wang; Weizhong Chen; Yannan Wang; Zhaowei Wu; Na Tang; Yu Wang; Suwen Zhao; Jianhua Gan; Quanjiang Ji

    Cas9 nucleases recognize and cleave their target DNA through base pairing of a guide RNA with a spacer adjacent to a protospacer adjacent motif (PAM). Streptococcus thermophilus Cas9 (St1Cas9), a smaller Cas9 orthologue than Streptococcus pyogenes Cas9, enables robust genome editing in diverse organisms. Here we report high-resolution structures of St1Cas9 in complex with a single-guide RNA and different

    更新日期:2020-09-08
  • Highly active and stable stepped Cu surface for enhanced electrochemical CO 2 reduction to C 2 H 4
    Nat. Catal. (IF 30.471) Pub Date : 2020-09-07
    Chungseok Choi; Soonho Kwon; Tao Cheng; Mingjie Xu; Peter Tieu; Changsoo Lee; Jin Cai; Hyuck Mo Lee; Xiaoqing Pan; Xiangfeng Duan; William A. Goddard; Yu Huang

    Electrochemical CO2 reduction to value-added chemical feedstocks is of considerable interest for renewable energy storage and renewable source generation while mitigating CO2 emissions from human activity. Copper represents an effective catalyst in reducing CO2 to hydrocarbons or oxygenates, but it is often plagued by a low product selectivity and limited long-term stability. Here we report that copper

    更新日期:2020-09-08
  • A fundamental look at electrocatalytic sulfur reduction reaction
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-31
    Lele Peng; Ziyang Wei; Chengzhang Wan; Jing Li; Zhuo Chen; Dan Zhu; Daniel Baumann; Haotian Liu; Christopher S. Allen; Xiang Xu; Angus I. Kirkland; Imran Shakir; Zeyad Almutairi; Sarah Tolbert; Bruce Dunn; Yu Huang; Philippe Sautet; Xiangfeng Duan

    The fundamental kinetics of the electrocatalytic sulfur reduction reaction (SRR), a complex 16-electron conversion process in lithium–sulfur batteries, is so far insufficiently explored. Here, by directly profiling the activation energies in the multistep SRR, we reveal that the initial reduction of sulfur to the soluble polysulfides is relatively easy owing to the low activation energy, whereas the

    更新日期:2020-09-01
  • Phase segregation reversibility in mixed-metal hydroxide water oxidation catalysts
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-24
    Chunguang Kuai; Zhengrui Xu; Cong Xi; Anyang Hu; Zhijie Yang; Yan Zhang; Cheng-Jun Sun; Luxi Li; Dimosthenis Sokaras; Cunku Dong; Shi-Zhang Qiao; Xi-Wen Du; Feng Lin

    Achieving stable, low-cost electrocatalysts represents a daunting challenge towards practical water oxidation reactions. Here, we report that a degraded electrocatalyst can be revivified under catalytic operating conditions by manipulating reversible phase segregation. Under the oxygen evolution reaction conditions, Fe segregation develops in the Ni–Fe hydroxide host lattice, with the formation of

    更新日期:2020-08-25
  • Structure dependency of the atomic-scale mechanisms of platinum electro-oxidation and dissolution
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-24
    Timo Fuchs; Jakub Drnec; Federico Calle-Vallejo; Natalie Stubb; Daniel J. S. Sandbeck; Martin Ruge; Serhiy Cherevko; David A. Harrington; Olaf M. Magnussen

    Platinum dissolution and restructuring due to surface oxidation are primary degradation mechanisms that limit the lifetime of platinum-based electrocatalysts for electrochemical energy conversion. Here, we have studied well-defined Pt(100) and Pt(111) electrode surfaces by in situ high-energy surface X-ray diffraction, online inductively coupled plasma mass spectrometry and density functional theory

    更新日期:2020-08-25
  • 19 F- and 18 F-arene deoxyfluorination via organic photoredox-catalysed polarity-reversed nucleophilic aromatic substitution
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-24
    Nicholas E. S. Tay; Wei Chen; Alison Levens; Vincent A. Pistritto; Zeng Huang; Zhanhong Wu; Zibo Li; David A. Nicewicz

    Nucleophilic aromatic substitution (SNAr) is routinely used to install 19F– and 18F– in aromatic molecules, but is typically limited to electron-deficient arenes due to kinetic barriers associated with C–F bond formation. Here we demonstrate that a polarity-reversed photoredox-catalysed arene deoxyfluorination that operates via cation-radical-accelerated SNAr enables the fluorination of electron-rich

    更新日期:2020-08-25
  • Tunable catalysis via insulator–metal transition
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-14
    Yifei Sun; Shriram Ramanathan

    Suppressing the degradation of polymer electrolyte membrane fuel cells due to anode side-reactions during repetitive cell start-up/shut-down remains a formidable challenge. Now, a phase transition material of WO3 has been explored as a smart catalytic switch to enable highly selective electrocatalysis and improve fuel cell longevity.

    更新日期:2020-08-14
  • Recommended practice to report selectivity in electrochemical synthesis of H 2 O 2
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-14
    Chuan Xia; Jung Yoon (Timothy) Kim; Haotian Wang

    Two different types of H2O2 selectivity are reported for the electrochemical synthesis of H2O2: molar fraction selectivity and Faradaic selectivity. Here we revisit their definitions and discuss the best way to report H2O2 selectivity, which can help to avoid misunderstandings or unfair performance comparisons in this growing field.

    更新日期:2020-08-14
  • Construction of axial chirality via palladium/chiral norbornene cooperative catalysis
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-10
    Ze-Shui Liu; Yu Hua; Qianwen Gao; Yuanyuan Ma; Hua Tang; Yong Shang; Hong-Gang Cheng; Qianghui Zhou

    Axially chiral biaryls are common structural motifs in functional materials, bioactive natural products, pharmaceuticals and chiral catalysts/ligands. As such, efficient preparation of these privileged scaffolds is an important endeavour in organic chemistry. Herein we report a general and modular platform technology for the construction of axial chirality via palladium/chiral norbornene cooperative

    更新日期:2020-08-10
  • Author Correction: Enantioselective hydrogenation of dialkyl ketones
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-04
    Feng-Hua Zhang; Fa-Jian Zhang; Mao-Lin Li; Jian-Hua Xie; Qi-Lin Zhou

    An amendment to this paper has been published and can be accessed via a link at the top of the paper.

    更新日期:2020-08-05
  • Author Correction: Tuning of catalytic sites in Pt/TiO 2 catalysts for the chemoselective hydrogenation of 3-nitrostyrene
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-03
    Margherita Macino; Alexandra J. Barnes; Sultan M. Althahban; Ruiyang Qu; Emma K. Gibson; David J. Morgan; Simon J. Freakley; Nikolaos Dimitratos; Christopher J. Kiely; Xiang Gao; Andrew M. Beale; Donald Bethell; Qian He; Meenakshisundaram Sankar; Graham J. Hutchings

    An amendment to this paper has been published and can be accessed via a link at the top of the paper.

    更新日期:2020-08-04
  • Author Correction: Selective electrocatalysis imparted by metal–insulator transition for durability enhancement of automotive fuel cells
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-03
    Sang-Mun Jung; Su-Won Yun; Jun-Hyuk Kim; Sang-Hoon You; Jinheon Park; Seonggyu Lee; Seo Hyoung Chang; Seung Chul Chae; Sang Hoon Joo; Yousung Jung; Jinwoo Lee; Junwoo Son; Joshua Snyder; Vojislav Stamenkovic; Nenad M. Markovic; Yong-Tae Kim

    An amendment to this paper has been published and can be accessed via a link at the top of the paper.

    更新日期:2020-08-04
  • Electrolytic deuteration of unsaturated bonds without using D 2
    Nat. Catal. (IF 30.471) Pub Date : 2020-08-03
    Aiko Kurimoto; Rebecca S. Sherbo; Yang Cao; Nicholas W. X. Loo; Curtis P. Berlinguette

    Site-selective deuteration of C–H bonds increases the lifetime and efficacy of drug molecules. Although effective methods to form C(sp2)–D bonds are known, processes for making C(sp3)–D bonds often have low site selectivity, require expensive and unrecoverable D2 gas, or use stoichiometric reagents. Here we report cost-efficient and site-selective reductive deuteration using a tandem electrochemical

    更新日期:2020-08-03
  • Creation of negatively curved polyaromatics enabled by annulative coupling that forms an eight-membered ring
    Nat. Catal. (IF 30.471) Pub Date : 2020-07-27
    Satoshi Matsubara; Yoshito Koga; Yasutomo Segawa; Kei Murakami; Kenichiro Itami

    The discoveries of new forms of carbon have always opened doors to new science and technology. In 1991, three-dimensional (3D) periodic carbon crystals with negative Gaussian curvatures that consist of six- and eight-membered rings were proposed. To realize these 3D periodic carbon crystals (known as Mackay crystals), methods for creating polyaromatic structures embedding eight-membered rings must

    更新日期:2020-07-28
  • Tuning water reduction through controlled nanoconfinement within an organic liquid matrix
    Nat. Catal. (IF 30.471) Pub Date : 2020-07-27
    Nicolas Dubouis; Alessandra Serva; Roxanne Berthin; Guillaume Jeanmairet; Benjamin Porcheron; Elodie Salager; Mathieu Salanne; Alexis Grimaud

    The growing hydrogen economy requires accelerating the hydrogen evolution reaction. The water dissociation step (Volmer step) has been proposed as a main kinetic limitation, but the mechanisms at play in the electrochemical double-layer are poorly understood. This is due to the dual role of water: it acts both as a reactant and as a solvent. Here we propose to confine water inside an organic liquid

    更新日期:2020-07-28
  • An artificial pathway for polyketide biosynthesis
    Nat. Catal. (IF 30.471) Pub Date : 2020-07-17
    Anuran K. Gayen; Lindsay Nichols; Gavin J. Williams

    Polyketide synthases are multi-domain enzymes that catalyse the construction of many bioactive natural products. Now, some of the inefficiencies and limitations of these systems have been solved by designing an artificial pathway for carbon–carbon bond formation via iterative rounds of non-decarboxylative thio-Claisen reactions.

    更新日期:2020-07-17
  • From desktop to benchtop with automated computational workflows for computer-aided design in asymmetric catalysis
    Nat. Catal. (IF 30.471) Pub Date : 2020-07-17
    Mihai Burai Patrascu; Joshua Pottel; Sharon Pinus; Michelle Bezanson; Per-Ola Norrby; Nicolas Moitessier

    The organic chemist’s toolbox is vast, with technologies to accelerate the synthesis of novel chemical matter. The field of asymmetric catalysis is one approach to accessing new areas of chemical space and computational power is today sufficient to assist in this exploration. Unfortunately, existing techniques generally require computational expertise and are therefore underutilized in synthetic chemistry

    更新日期:2020-07-17
  • Palladium-catalysed cross-coupling of lithium acetylides
    Nat. Catal. (IF 30.471) Pub Date : 2020-07-13
    Hugo Helbert; Paco Visser; Johannes G. H. Hermens; Jeffrey Buter; Ben L. Feringa

    The incorporation of alkynes into organic molecules is one of the most valuable transformations for the formation of C–C bonds and provides a versatile handle for further modifications. The Sonogashira cross-coupling of acetylenes holds a prominent position among the suite of catalytic cross-coupling reactions that are key to modern synthesis. Here we present a method that is complementary to the Sonogashira

    更新日期:2020-07-13
  • Alkali ions secure hydrides for catalytic hydrogenation
    Nat. Catal. (IF 30.471) Pub Date : 2020-07-13
    Ruixuan Qin; Lingyun Zhou; Pengxin Liu; Yue Gong; Kunlong Liu; Chaofa Xu; Yun Zhao; Lin Gu; Gang Fu; Nanfeng Zheng

    Catalytic hydrogenation is one of the backbones of the chemical industry. Controlling the reaction behaviour of the activated hydrogen species over oxide-supported metal catalysts is essential. Aside from the expected addition to substrates, the activated hydrogen species would also destroy the active structures. Here we show that, with the assistance of alkali cations, the atomically dispersed Ru(iii)

    更新日期:2020-07-13
  • Overcoming limitations in dual photoredox/nickel-catalysed C–N cross-couplings due to catalyst deactivation
    Nat. Catal. (IF 30.471) Pub Date : 2020-07-06
    Sebastian Gisbertz; Susanne Reischauer; Bartholomäus Pieber

    Dual photoredox/nickel-catalysed C–N cross-couplings suffer from low yields for electron-rich aryl halides. The formation of catalytically inactive nickel-black is responsible for this limitation and causes severe reproducibility issues. Here, we demonstrate that catalyst deactivation can be avoided by using a carbon nitride photocatalyst. The broad absorption of the heterogeneous photocatalyst enables

    更新日期:2020-07-06
  • Selective electrocatalysis imparted by metal–insulator transition for durability enhancement of automotive fuel cells
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-29
    Sang-Mun Jung; Su-Won Yun; Jun-Hyuk Kim; Sang-Hoon You; Jinheon Park; Seonggyu Lee; Seo Hyoung Chang; Seung Chul Chae; Sang Hoon Joo; Yousung Jung; Jinwoo Lee; Junwoo Son; Joshua Snyder; Vojislav Stamenkovic; Nenad M. Markovic; Yong-Tae Kim

    Repetitive start-up and shut-down events in polymer electrolyte membrane fuel cells for automotive applications lead to serious corrosion of the cathode due to an instantaneous potential jump that results from unintended air leakage into the anodic flow field followed by a parasitic oxygen reduction reaction (ORR) on the anode. Here we report a solution to the cathode corrosion issue during the start-up/shut-down

    更新日期:2020-06-30
  • Molecular-level insights on the reactive facet of carbon nitride single crystals photocatalysing overall water splitting
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-29
    Lihua Lin; Zhiyou Lin; Jian Zhang; Xu Cai; Wei Lin; Zhiyang Yu; Xinchen Wang

    Unraveling how reactive facets promote photocatalysis at the molecular level remains a grand challenge, while identification of the reactive facets can provide guidelines for designing highly efficient photocatalysts and unravelling the microscopic mechanisms behind them. Recently, a series of polytriazine imides (PTIs) was reported with highly crystalline structures; all had a relatively low photocatalytic

    更新日期:2020-06-30
  • Chance emergence of catalytic activity and promiscuity in a self-replicator
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-26
    Jim Ottelé; Andreas S. Hussain; Clemens Mayer; Sijbren Otto

    How life can emerge from inanimate matter is one of the grand questions in science. Self-replicating molecules are necessary for the transition from chemistry to biology, but they need to acquire additional functions for life to emerge. Catalysis is one of the most essential of such functionalities, but mechanisms through which self-replicators can acquire catalytic and, in extension, metabolic properties

    更新日期:2020-06-26
  • Enantioselective hydrogenation of dialkyl ketones
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-22
    Feng-Hua Zhang; Fa-Jian Zhang; Mao-Lin Li; Jian-Hua Xie; Qi-Lin Zhou

    Chiral catalyst development is a key to asymmetric catalysis research. The enantioselectivity of a chiral catalyst relies on its ability to distinguish the prochiral centres or faces of substrates, which is difficult when the two groups attached to the centre or face are spatially and electronically similar. For example, dialkyl ketones are difficult to reduce enantioselectively. Here we report a protocol

    更新日期:2020-06-23
  • Structural modulation and direct measurement of subnanometric bimetallic PtSn clusters confined in zeolites
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-22
    Lichen Liu; Miguel Lopez-Haro; Christian W. Lopes; Sergio Rojas-Buzo; Patricia Concepcion; Ramón Manzorro; Laura Simonelli; Aaron Sattler; Pedro Serna; Jose J. Calvino; Avelino Corma

    Modulating the structures of subnanometric metal clusters at the atomic level is a great synthetic and characterization challenge in catalysis. Here, we show how the catalytic properties of subnanometric platinum clusters (0.5–0.6 nm) confined in the sinusoidal 10R channels of purely siliceous MFI zeolite are modulated upon introduction of partially reduced tin species that interact with the noble

    更新日期:2020-06-23
  • A polyketoacyl-CoA thiolase-dependent pathway for the synthesis of polyketide backbones
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-22
    Zaigao Tan; James M. Clomburg; Seokjung Cheong; Shuai Qian; Ramon Gonzalez

    Polyketides found in nature originate from backbones synthesized through iterative decarboxylative Claisen condensations catalysed by polyketide synthases (PKSs). However, PKSs suffer from complicated architecture, energy inefficiencies, complex regulation, and competition with essential metabolic pathways for extender unit malonyl-CoA, all combining to limit the flux of polyketide biosynthesis. Here

    更新日期:2020-06-23
  • Cycling back to biocatalysis
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-18
    Mohamed A. Attia; Christopher J. Thibodeaux

    Macrocyclic peptide natural products are important medicinal compounds. The catalytic properties of an unusual peptide cyclase enzyme have recently been described — providing opportunities for the engineering and synthesis of structurally complex peptides with novel biological activities.

    更新日期:2020-06-18
  • Of best practice in catalysis
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-18

    Reporting data according to standards accepted by the community is fundamental to the progress of science. In the broad area of catalysis, best practice principles are well consolidated in some subfields, but they are still developing in others.

    更新日期:2020-06-18
  • Boosting chemical and fuel production
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-18
    Cao-Thang Dinh

    Catalysts are the heart of CO2 electroreduction technology. Now, a catalyst has been developed that converts CO2 into C2+ products with very high selectivity, stability, and energy efficiency at industrially relevant current densities.

    更新日期:2020-06-18
  • Covalency competition dominates the water oxidation structure–activity relationship on spinel oxides
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-15
    Yuanmiao Sun; Hanbin Liao; Jiarui Wang; Bo Chen; Shengnan Sun; Samuel Jun Hoong Ong; Shibo Xi; Caozheng Diao; Yonghua Du; Jia-Ou Wang; Mark B. H. Breese; Shuzhou Li; Hua Zhang; Zhichuan J. Xu

    Spinel oxides have attracted growing interest over the years for catalysing the oxygen evolution reaction (OER) due to their efficiency and cost-effectiveness, but fundamental understanding of their structure–property relationships remains elusive. Here we demonstrate that the OER activity on spinel oxides is intrinsically dominated by the covalency competition between tetrahedral and octahedral sites

    更新日期:2020-06-15
  • Publisher Correction: Asymmetric O -propargylation of secondary aliphatic alcohols
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-08
    Ren-Zhe Li; Da-Qi Liu; Dawen Niu

    An amendment to this paper has been published and can be accessed via a link at the top of the paper.

    更新日期:2020-06-08
  • Site-selective alkene borylation enabled by synergistic hydrometallation and borometallation
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-08
    Xiaolong Yu; Haonan Zhao; Shibo Xi; Zhongxin Chen; Xiaowei Wang; Lin Wang; Leroy Qi Hao Lin; Kian Ping Loh; Ming Joo Koh

    The selective installation of boryl units at less-activated sites, which will facilitate easy access to a range of core structures embedded within bioactive molecules, is a longstanding challenge. Here, we show that catalytic amounts of an earth-abundant Fe(ii)-based complex promote efficient borylations at typically less-reactive positions vicinal (β) to common functional units. Utility is highlighted

    更新日期:2020-06-08
  • Plasmon-driven carbon–fluorine (C( sp 3 )–F) bond activation with mechanistic insights into hot-carrier-mediated pathways
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-08
    Hossein Robatjazi; Junwei Lucas Bao; Ming Zhang; Linan Zhou; Phillip Christopher; Emily A. Carter; Peter Nordlander; Naomi J. Halas

    The activation of carbon–fluorine bonds is an industrially and environmentally critical, but energetically challenging, transformation. Here we demonstrate a plasmonic photocatalysis approach to visible-light-driven hydrodefluorination that utilizes aluminium–palladium antenna–reactor heterostructures. Photocatalytic hydrodefluorination of aliphatic carbon–fluorine (C(sp3)–F) bonds in fluoromethane

    更新日期:2020-06-08
  • Asymmetric O -propargylation of secondary aliphatic alcohols
    Nat. Catal. (IF 30.471) Pub Date : 2020-06-01
    Ren-Zhe Li; Da-Qi Liu; Dawen Niu

    The asymmetric O-alkylation of secondary aliphatic alcohols remains a substantial challenge in chemistry. Such a challenge largely stems from the steric demand of each reactant, in addition to the relatively low nucleophilicity of alcohols. Here, we report the development of a base-free, Cu-catalysed propargylic substitution reaction that enables the efficient, asymmetric O-propargylation of secondary

    更新日期:2020-06-01
  • Electrode design for ammonia synthesis
    Nat. Catal. (IF 30.471) Pub Date : 2020-05-20
    Claudio Ampelli

    A rapid and efficient electrochemical reaction requires active catalytic material, as well as proper electrode and cell design. Now, a gas diffusion electrode based on a stainless steel cloth successfully overcomes gas transport limitations for high-current ammonia electrosynthesis in non-aqueous solvents at ambient conditions.

    更新日期:2020-05-20
  • Fungal-derived brevianamide assembly by a stereoselective semipinacolase.
    Nat. Catal. (IF 30.471) Pub Date : 2020-05-18
    Ying Ye,Lei Du,Xingwang Zhang,Sean A Newmister,Morgan McCauley,Juan V Alegre-Requena,Wei Zhang,Shuai Mu,Atsushi Minami,Amy E Fraley,Maria L Adrover-Castellano,Nolan A Carney,Vikram V Shende,Feifei Qi,Hideaki Oikawa,Hikaru Kato,Sachiko Tsukamoto,Robert S Paton,Robert M Williams,David H Sherman,Shengying Li

    Fungal bicyclo[2.2.2]diazaoctane indole alkaloids represent an important family of natural products with a wide spectrum of biological activities. Although biomimetic total syntheses of representative compounds have been reported, the details of their biogenesis, especially the mechanisms for the assembly of diastereomerically distinct and enantiomerically antipodal metabolites, have remained largely

    更新日期:2020-05-18
  • Cu-catalysed intramolecular radical enantioconvergent tertiary β-C( sp 3 )–H amination of racemic ketones
    Nat. Catal. (IF 30.471) Pub Date : 2020-05-18
    Chang-Jiang Yang; Chi Zhang; Qiang-Shuai Gu; Jia-Heng Fang; Xiao-Long Su; Liu Ye; Yan Sun; Yu Tian; Zhong-Liang Li; Xin-Yuan Liu

    In contrast to the wealth of enantioselective prochiral C(sp3)–H functionalization that is transition-metal-catalysed, the enantioconvergent transformation of racemic tertiary C(sp3)–H bonds (pKa > 25) still represents a vastly uncharted domain. The mechanistic limitation is partial or complete chirality retention, which is inherent to developed enantioselective C–H functionalization catalysis and

    更新日期:2020-05-18
  • Boosting CO 2 hydrogenation via size-dependent metal–support interactions in cobalt/ceria-based catalysts
    Nat. Catal. (IF 30.471) Pub Date : 2020-05-11
    Alexander Parastaev; Valery Muravev; Elisabet Huertas Osta; Arno J. F. van Hoof; Tobias F. Kimpel; Nikolay Kosinov; Emiel J. M. Hensen

    Metal–support interactions have a strong impact on the performance of heterogeneous catalysts. Specific sites at the metal–support interface can give rise to unusual high reactivity, and there is a growing interest in optimizing not only the properties of metal particles but also the metal–support interface. Here, we demonstrate how varying the particle size of the support (ceria–zirconia) can be used

    更新日期:2020-05-11
  • Operando identification of site-dependent water oxidation activity on ruthenium dioxide single-crystal surfaces
    Nat. Catal. (IF 30.471) Pub Date : 2020-05-11
    Reshma R. Rao; Manuel J. Kolb; Livia Giordano; Anders Filsøe Pedersen; Yu Katayama; Jonathan Hwang; Apurva Mehta; Hoydoo You; Jaclyn R. Lunger; Hua Zhou; Niels Bendtsen Halck; Tejs Vegge; Ib Chorkendorff; Ifan E. L. Stephens; Yang Shao-Horn

    Understanding the nature of active sites is central to controlling (electro)catalytic activity. Here we employed surface X-ray scattering coupled with density functional theory and surface-enhanced infrared absorption spectroscopy to examine the oxygen evolution reaction on RuO2 surfaces as a function of voltage. At 1.5 VRHE, our results suggest that there is an –OO group on the coordinatively unsaturated

    更新日期:2020-05-11
  • Non-aqueous gas diffusion electrodes for rapid ammonia synthesis from nitrogen and water-splitting-derived hydrogen
    Nat. Catal. (IF 30.471) Pub Date : 2020-05-04
    Nikifar Lazouski; Minju Chung; Kindle Williams; Michal L. Gala; Karthish Manthiram

    Electrochemical transformations in non-aqueous solvents are important for synthetic and energy storage applications. Use of non-polar gaseous reactants such as nitrogen and hydrogen in non-aqueous solvents is limited by their low solubility and slow transport. Conventional gas diffusion electrodes improve the transport of gaseous species in aqueous electrolytes by facilitating efficient gas–liquid

    更新日期:2020-05-04
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