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Selective CO2 Reduction to Formate on a Zn-Based Electrocatalyst Promoted by Tellurium
Chemistry of Materials ( IF 8.6 ) Pub Date : 2022-06-22 , DOI: 10.1021/acs.chemmater.2c01131
Xue Teng 1 , Jianmin Lu 2 , Yanli Niu 1 , Shuaiqi Gong 1 , Mingze Xu 1 , Thomas J. Meyer 3 , Zuofeng Chen 1
Affiliation  

Zn-based materials represent a class of low-cost, promising electrocatalysts for CO2 reduction but the tuning of catalytic activity and selectivity by varying composition and nanostructure is a challenge. Herein, a ZnTe/ZnO heterostructured material supported on N-doped carbon nanosheets (ZnTe/ZnO@C) is prepared with a novel ZnTe metal–organic framework (MOF). The hybrid material exhibits greatly enhanced performances for CO2 reduction to formate with a sustained current density of 16 mA cm–2 and a selectivity of 86% at −1.1 V vs reversible hydrogen electrode (RHE) in bicarbonate solutions. The observation of Te-promoted CO2 reduction to formate, with high activity and selectivity, is notable in contrast to other Zn-based electrocatalysts. Density functional theory (DFT) analysis implies that selective formate formation is promoted by the stabilization of the key HCOO* intermediate on ZnTe. Additionally, ZnTe/ZnO@C is also an excellent catalyst for oxygen evolution owing to its high electrical conductivity and the high degree of covalency in ZnTe. The bifunctionality of ZnTe/ZnO@C toward both reactions is demonstrated by assembling a two-electrode electrochemical cell for CO2/H2O splitting and a fascinating rechargeable Zn–CO2 battery. The latter, when constructed with ZnTe/ZnO@C as the cathode and Zn foil as the anode, yields a Zn–CO2 battery fully based on Zn-based materials.

中文翻译:

碲促进的锌基电催化剂选择性 CO2 还原生成甲酸盐

锌基材料代表了一类低成本、有前途的 CO 2还原电催化剂,但通过改变成分和纳米结构来调节催化活性和选择性是一个挑战。在此,利用新型 ZnTe 金属有机框架 (MOF) 制备了负载在 N 掺杂碳纳米片 (ZnTe/ZnO@C) 上的 ZnTe/ZnO 异质结构材料。该杂化材料在 CO 2还原生成甲酸盐方面表现出显着增强的性能,在碳酸氢盐溶液中具有 16 mA cm –2的持续电流密度和 86% 的选择性(-1.1 V可逆氢电极 (RHE) 相比)。Te促进CO 2的观察与其他锌基电催化剂相比,还原成甲酸盐具有高活性和选择性。密度泛函理论 (DFT) 分析表明选择性甲酸盐的形成是通过稳定 ZnTe 上的关键 HCOO* 中间体来促进的。此外,由于 ZnTe/ZnO@C 的高导电性和 ZnTe 中的高度共价性,它也是一种优异的析氧催化剂。通过组装用于 CO 2 /H 2 O 分解的双电极电化学电池和迷人的可充电 Zn-CO 2电池,证明了 ZnTe/ZnO@C 对这两种反应的双功能。后者,当以 ZnTe/ZnO@C 作为阴极和 Zn 箔作为阳极时,产生 Zn-CO 2完全基于锌基材料的电池。
更新日期:2022-06-22
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