本研究表明,在脉冲模式电解过程中,将银结合到氧化物衍生的铜上有助于CO转化为醇,其选择性为75.7%,其中正丙醇的选择性为48.8%。选择性增强的基础似乎是可调的氢氧化物表面吸附,由Ag和脉冲协同作用,平衡了结合的CO构型,以及氢与界面水结合程度的降低,有利于Langmuir-Hinshelwood加氢途径。将催化剂集成在连续流电解槽的阴极上,阳极为氢氧化,在116 h的时间内将CO还原为多碳醇,法拉第效率为66.7%(其中正丙醇为40.4%)。对关键中间体吸附构型和界面水结构的相干控制将推进乙醇生产的电化学转化技术。
据了解,电化学还原二氧化碳和一氧化碳(CO)为生产高价值醇(如正丙醇)提供了有希望的方法,但高效和选择性转化需要改进的催化剂。
附:英文原文
Title: Selective CO Conversion to Multicarbon Alcohols via Balancing Adsorbate Configurations
Author: Shu-Ping Sun, Xiao-Long Zhang, Xue-Peng Yang, Peng-Cheng Yu, Ye-Cheng Li, Yu-Cai Zhang, Pu-Gan Lu, Yu Yang, Ye-Hua Wang, Lei Zhu, Hui-Kun Yan, Tian-Yun Zhang, Wen-Long Liang, Tao Fang, Min-Rui Gao
Issue&Volume: December 2, 2025
Abstract: Electrochemical carbon dioxide and carbon monoxide (CO) reductions offer promising ways to produce high-value alcohols, such as n-propanol, but efficient and selective conversion requires improved catalysts. Here we show that incorporating silver onto oxide-derived copper facilitates the conversion of CO to alcohols with 75.7% selectivity, including 48.8% toward n-propanol, during pulsed-mode electrolysis. The basis for the selectivity enhancements appears to be the tunable hydroxide surface adsorption enabled synergistically by Ag and pulsing, which balances the bound CO configurations, as well as the decreased degree of hydrogen binding to interfacial water that benefits the Langmuir–Hinshelwood hydrogenation route. For illustration, the catalyst was integrated into the cathode of a continuous-flow electrolyzer operating with hydrogen oxidation at the anode, which reduced CO to multicarbon alcohols with a Faradaic efficiency of 66.7% (including 40.4% n-propanol) over the course of 116 h. The coherent control over the adsorption configuration of key intermediates and the interfacial water structure will advance electrochemical conversion technology for alcohol production.
DOI: 10.1021/jacs.5c15536
Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c15536
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
官方网址:https://pubs.acs.org/journal/jacsat
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