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一种精确调控一氧化碳电还原中合成气组成的创新方法。

An Innovative Approach to Precisely Tailor the Composition of Syngas in CO Electroreduction.

作者信息

Lv Shuai, Sun Xinyi, Wang Baolin, Wan Wenrui, Wang Li, Wang Jianji, Zhang Jinglai

机构信息

Henan Key Laboratory of Protection and Safety Energy Storage of Light Metal Materials, College of Chemistry and Molecular Sciences, Henan University, Kaifeng, Henan, 475004, P. R. China.

Key Laboratory of Green Chemical Media and Reactions (Ministry of Education), Collaborative Innovation Centre of Henan Province for Green Manufacturing of Fine Chemicals, School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, Henan, 453007, P. R. China.

出版信息

Adv Sci (Weinh). 2025 Jun 23:e05424. doi: 10.1002/advs.202505424.

Abstract

Syngas production through CO electrochemical reduction reaction (CORR) has attracted numerous attention for reducing carbon emissions and increasing chemical feedstocks. However, the precise regulation of H/CO molar ratio in syngas remains a challenge, especially through simple and feasible methodologies. In this work, a novel composite electrocatalyst, copper-indium/black phosphorus (CuIn/BP) is developed, using a simple one-step co-reduction method for efficient CORR. It is found for the first time that there is a linear relationship between BP content in CuIn/BP and the H/CO molar ratio in syngas. Consequently, the H/CO molar ratio in syngas can be precisely tailored by simply adjusting the BP content in CuIn/BP. A total faradaic efficiency (FE) of CO and H reached ≈ 100% along with a current density of 135.2 mA cm. Mechanistic studies suggest that the CuIn phase and CuP species are in situ generated in CuIn/BP, where the CuIn phases mainly contribute to CO generation, while the CuP species promote H formation. The variation in BP content modulates the proportion of the CuIn phase and CuP species, leading to the variations in H/CO molar ratios. Thus, this study provides an efficient and simple strategy to tailor the H/CO molar ratio in syngas for various industrial applications.

摘要

通过CO电化学还原反应(CORR)生产合成气在减少碳排放和增加化学原料方面引起了广泛关注。然而,精确调控合成气中H/CO摩尔比仍然是一项挑战,特别是通过简单可行的方法来实现。在这项工作中,采用简单的一步共还原法开发了一种新型复合电催化剂铜铟/黑磷(CuIn/BP)用于高效CORR。首次发现CuIn/BP中BP含量与合成气中H/CO摩尔比之间存在线性关系。因此,通过简单调节CuIn/BP中的BP含量就可以精确调整合成气中的H/CO摩尔比。CO和H的总法拉第效率(FE)达到≈100%,同时电流密度为135.2 mA/cm。机理研究表明,CuIn相和CuP物种在CuIn/BP中原位生成,其中CuIn相主要促进CO生成,而CuP物种促进H的形成。BP含量的变化调节了CuIn相和CuP物种的比例,导致H/CO摩尔比的变化。因此,本研究提供了一种有效且简单的策略,可针对各种工业应用调整合成气中的H/CO摩尔比。

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