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Reconstruction-induced NiCu-based catalysts towards paired electrochemical refining
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2022-05-12 , DOI: 10.1039/d2ee00461e
Shanlin Li 1, 2, 3 , Peijie Ma 2 , Chunlang Gao 2 , Lijia Liu 4 , Xunlu Wang 1, 3 , Mohsen Shakouri 5 , Roman Chernikov 5 , Kaiwen Wang 2 , Danmin Liu 2 , Ruguang Ma 6 , Jiacheng Wang 1, 3, 7
Affiliation  

A paired electrochemical refinery toward the cathodic nitrate reduction reaction (NO3RR) and anodic glycerol oxidation reaction (GOR) driven by renewable electricity could generate high value-added ammonia and formic acid simultaneously. However, both cathode and anode electrocatalysts often suffer from low efficiency and unclear reconstruction. Herein, we prepare a non-noble NiCu–OH nanocomposite precatalyst composed of crystalline Cu2(OH)3(NO3) and amorphous Ni(OH)2, which can be reconstructed into high-activity and stable cathodic NO3RR and anodic GOR electrocatalysts under operating conditions. Various in situ and ex situ experiments demonstrate that NiCu–OH could convert into active Cu nanoparticles coupled with amorphous Ni(OH)2 under cathodic NO3RR conditions. Meanwhile, under anodic GOR conditions, NiCu–OH-derived bimetal oxide (NiCuO) changes into active NiOOH species composited with Cu vacancy-rich CuO. Furthermore, an actual paired electrochemical refinery with the reconstructed NiCu-based catalysts toward the NO3RR and GOR shows a low potential of 1.37 V at a current density of 100 mA cm−2 to continuously produce ammonium and formate. This study provides a new paradigm for the design of an electrochemical refinery with reconstructed non-noble electrocatalysts toward chemical upgradation.

中文翻译:

用于配对电化学精炼的重构诱导 NiCu 基催化剂

由可再生电力驱动的阴极硝酸盐还原反应(NO 3 RR)和阳极甘油氧化反应(GOR)的配对电化学炼油厂可以同时产生高附加值的氨和甲酸。然而,阴极和阳极电催化剂通常都存在效率低和重构不明确的问题。在此,我们制备了一种由结晶Cu 2 (OH) 3 (NO 3 ) 和无定形Ni(OH) 2组成的非贵金属NiCu-OH纳米复合预催化剂,可将其重构为高活性且稳定的阴极NO 3 RR和阳极运行条件下的 GOR 电催化剂。各种原位异位实验表明,在阴极 NO 3 RR 条件下,NiCu-OH 可以转化为与无定形 Ni(OH) 2偶联的活性 Cu 纳米颗粒。同时,在阳极 GOR 条件下,NiCu-OH 衍生的双金属氧化物 (NiCuO) 转变为与富含 Cu 空位的 CuO 复合的活性 NiOOH 物种。此外,一个实际配对的电化学精炼厂与针对 NO 3 RR 和 GOR的重构 NiCu 基催化剂在 100 mA cm -2的电流密度下显示出 1.37 V 的低电位,以连续生产铵和甲酸盐。该研究为电化学精炼厂的设计提供了一种新的范式,该精炼厂采用重构的非贵金属电催化剂进行化学升级。
更新日期:2022-05-12
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