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A Trimetallic Cu(II) Derivative as an Efficient and Stable Electrocatalyst for Reduction of Proton to Molecular Hydrogen
Catalysis Letters ( IF 2.3 ) Pub Date : 2020-02-21 , DOI: 10.1007/s10562-020-03150-x
Kuheli Das , Belete B. Beyene , Amogne W. Yibeltal , Sanchita Goswami , Chiara Massera , Eugenio Garribba , Amitabha Datta , Chen-Hsiung Hung

A trinuclear copper(II) complex, namely [Cu 3 (L) 2 (CF 3 COO) 2 ] ( 1 ) is afforded integrating a ‘compartmental’ Schiff base, H 2 L [where H 2 L = N , N ′-bis(salicylidene)-1,3-propanediamine] and fully characterized. Complex 1 is implemented for electrocatalytic proton reduction to originate molecular hydrogen in a homogenous system. The electrochemical study involving CV (cyclic voltammetry), CPE (controlled potential electrolysis) and GC (gas chromatography) reveals that in homogeneous system, 1 is highly active towards proton reduction in presence of trifluoro acetic acid as a proton source. Following CPE at − 1.8 V vs Ag/AgCl, the headspace gas is sampled and gas chromatography is carried out to quantify the amount of hydrogen discharged. The ratio of theoretical H 2 production from charge aggregation during electrolysis to the practical amount of H 2 resolved on GC is yielded a Faradaic efficiency value of 87%. Moreover, an extended bulk electrolysis experiment carried out for 35 h illustrates the presence of a stable catalytic system in which 230 C of charge is accumulated. As a consequence, this efficient and stable H 2 evolution obtained using a Cu(II) derivative (Cu II is cheap and earth abundant) has shown that the synthesis of judiciously designed copper complex is a promising strategy towards potential catalysts from proton reduction. Graphic Abstract Electrochemical and catalytic study of a trimetallic Cu(II) derivative in DMSO with the presence of trifluoroacetic acid as weak proton source shows the hydrogen evolution Faradaic efficiency as 87%. A continuous increment of the charge accumulation through time is observed, indicating the high stability of our catalyst under electrochemical H2 generation.

中文翻译:

三金属 Cu(II) 衍生物作为一种高效且稳定的电催化剂,用于将质子还原为分子氢

三核铜(II) 络合物,即[Cu 3 (L) 2 (CF 3 COO) 2 ] ( 1 ) 被提供整合'室'希夫碱,H 2 L [其中H 2 L = N,N '-双(水杨基)-1,3-丙二胺]并充分表征。配合物 1 用于电催化质子还原以在均相系统中产生分子氢。涉及 CV(循环伏安法)、CPE(受控电位电解)和 GC(气相色谱法)的电化学研究表明,在均相系统中,1 在三氟乙酸作为质子源的情况下对质子还原具有高度活性。在 - 1.8 V vs Ag/AgCl 的 CPE 之后,对顶空气体进行采样,并进行气相色谱以量化排放的氢气量。电解过程中电荷聚集产生的理论 H 2 产量与 GC 解析的实际 H 2 量之比得出法拉第效率值为 87%。此外,进行了 35 小时的扩展本体电解实验表明存在稳定的催化系统,其中积累了 230 C 的电荷。因此,使用 Cu(II) 衍生物(Cu II 便宜且地球资源丰富)获得的这种高效且稳定的 H 2 析出表明,精心设计的铜配合物的合成是从质子还原中获得潜在催化剂的有前途的策略。图形摘要 在三氟乙酸作为弱质子源的情况下,三金属 Cu(II) 衍生物在 DMSO 中的电化学和催化研究表明,析氢法拉第效率为 87%。
更新日期:2020-02-21
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