“Two Ships in a Bottle” Design for Zn–Ag–O Catalyst Enabling Selective and Long-Lasting CO2 Electroreduction,Journal of the American Chemical Society

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“Two Ships in a Bottle” Design for Zn–Ag–O Catalyst Enabling Selective and Long-Lasting CO2 Electroreduction
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-04-14 , DOI: 10.1021/jacs.0c12418
Zhen Zhang ₁ , Guobin Wen ₁ , Dan Luo ₁ , Bohua Ren ₁ , Yanfei Zhu ₁ , Rui Gao ₁ , Haozhen Dou ₁ , Guiru Sun ₂ , Ming Feng ₂ , Zhengyu Bai ₃ , Aiping Yu ₁ , Zhongwei Chen ₁

Affiliation

Electrochemical CO₂ reduction (CO₂RR) using renewable energy sources represents a sustainable means of producing carbon-neutral fuels. Unfortunately, low energy efficiency, poor product selectivity, and rapid deactivation are among the most intractable challenges of CO₂RR electrocatalysts. Here, we strategically propose a “two ships in a bottle” design for ternary Zn–Ag–O catalysts, where ZnO and Ag phases are twinned to constitute an individual ultrafine nanoparticle impregnated inside nanopores of an ultrahigh-surface-area carbon matrix. Bimetallic electron configurations are modulated by constructing a Zn–Ag–O interface, where the electron density reconfiguration arising from electron delocalization enhances the stabilization of the *COOH intermediate favorable for CO production, while promoting CO selectivity and suppressing HCOOH generation by altering the rate-limiting step toward a high thermodynamic barrier for forming HCOO*. Moreover, the pore-constriction mechanism restricts the bimetallic particles to nanosized dimensions with abundant Zn–Ag–O heterointerfaces and exposed active sites, meanwhile prohibiting detachment and agglomeration of nanoparticles during CO₂RR for enhanced stability. The designed catalysts realize 60.9% energy efficiency and 94.1 ± 4.0% Faradaic efficiency toward CO, together with a remarkable stability over 6 days. Beyond providing a high-performance CO₂RR electrocatalyst, this work presents a promising catalyst-design strategy for efficient energy conversion.

中文翻译：

Zn-Ag-O催化剂的“两瓶装”设计可实现选择性和持久的CO ₂电还原

使用可再生能源的电化学CO ₂还原（CO ₂ RR）代表了一种生产碳中性燃料的可持续方式。不幸的是，低能效，较差的产品选择性和快速失活是CO ₂最棘手的挑战RR电催化剂。在这里，我们策略性地提出了一种用于三元Zn-Ag-O催化剂的“两瓶装”设计，其中ZnO和Ag相孪生在一起，构成了一个浸入超高表面积碳基质纳米孔内部的单个超细纳米颗粒。通过构造Zn–Ag–O界面来调节双金属电子构型，其中电子离域引起的电子密度重构增强了* COOH中间体的稳定性，从而有利于CO的产生，同时通过改变速率-促进了CO的选择性并抑制了HCOOH的产生。限制了向形成HCOO *的高热力学屏障的步伐。此外，孔收缩机制将双金属颗粒限制在具有丰富的Zn-Ag-O异质界面和暴露的活性位点的纳米尺寸上，₂ RR增强稳定性。设计的催化剂可实现60.9％的能源效率和94.1±4.0％的CO法拉第效率，并在6天之内具有出色的稳定性。除了提供高性能的CO ₂ RR电催化剂以外，这项工作还提出了一种有前途的催化剂设计策略，以实现高效的能量转换。

更新日期：2021-05-12

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