在拉伸应变 Ptδ+-Cuδ+ 双基点上原位揭示二氧化碳电还原的 C-C 耦合行为

IF 9.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Feng-Ya Ma, Pu Huang, Jing Zhou, Hong-Wei Zeng, Jia-Wei Zhang, Hui Zhao, Yu-Ming Dong, Yong-Fa Zhu, Yao Wang
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引用次数: 0

摘要

设计所需的双金属位点以实现 CO2 的 C-C 偶联对于 CO2 电还原反应(CER)的实际应用具有重要意义。本文提出了一种构建异质 Ptδ+-Cuδ+ 双位点的有效策略,以加强 CER 过程中 *CO 和 *CHO(或 *COH)的生成和耦合。半径更大的铂不仅能稳定 Cuδ+,还能在 Ptδ+-Cuδ+ 双位点中产生拉伸应变。获得的 Ptδ+-Cuδ+ 双位点在 - 1.20 V(相对于 RHE)电压下的总法拉第效应和 C2 产物的电流密度分别为 70.9% 和 586.9 mA-cm-2,高于 Cuδ+ 单位点(55.4%,286.9 mA-cm-2)。原位衰减全反射表面增强红外吸收光谱(ATR-SEIRAS)显示,Ptδ+-Cuδ+ 双位点可促进 C1 中间体(如 *CO、*COOH、*COH 和 *CHO)的生成和 C-C 耦合。其他原位表面增强拉曼光谱表明,Ptδ+-Cuδ+ 双位点可诱导 *COatop 高频峰的产生,从而加速 C-C 耦合。这项工作为稳定和提高 Cuδ+ 位点在 CER 方面的性能提供了一条很有前景的途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

In situ revealing C–C coupling behavior for CO2 electroreduction on tensile strain Ptδ+–Cuδ+ dual sites

In situ revealing C–C coupling behavior for CO2 electroreduction on tensile strain Ptδ+–Cuδ+ dual sites

Engineering the desired dual metal sites to realize C–C coupling of CO2 is of great importance for the practical applications of CO2 electroreduction reaction (CER). Herein, an efficient strategy for constructing heterogeneous Ptδ+–Cuδ+ dual sites to strengthen the generation and coupling of *CO and *CHO (or *COH) during CER process is presented in this work. The radii-larger Pt not only stabilizes the Cuδ+ but also induces a tensile strain in Ptδ+–Cuδ+ dual sites. The obtained Ptδ+–Cuδ+ dual sites achieve a total Faradaic efficiency and current density of C2 products with 70.9% and 586.9 mA·cm−2 at – 1.20 V (vs. RHE), which is higher than that of Cuδ+ single site (55.4%, 286.9 mA·cm−2). The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveals that the Ptδ+–Cuδ+ dual sites can promote the generation of C1 intermediates (such as *CO, *COOH, *COH, and *CHO) and C–C coupling. Additional in situ surface-enhanced Raman spectra demonstrate that Ptδ+–Cuδ+ dual sites can induce the generation of the high-frequency peak for *COatop, thus accelerating the C–C coupling. This work provides a promising avenue for stabilizing and enhancing the performance of Cuδ+ sites toward CER.

Graphical abstract

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来源期刊
Rare Metals
Rare Metals 工程技术-材料科学:综合
CiteScore
12.10
自引率
12.50%
发文量
2919
审稿时长
2.7 months
期刊介绍: Rare Metals is a monthly peer-reviewed journal published by the Nonferrous Metals Society of China. It serves as a platform for engineers and scientists to communicate and disseminate original research articles in the field of rare metals. The journal focuses on a wide range of topics including metallurgy, processing, and determination of rare metals. Additionally, it showcases the application of rare metals in advanced materials such as superconductors, semiconductors, composites, and ceramics.
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