Proton Shuttling by Polyaniline of High Brønsted Basicity for Improved Electrocatalytic Ethylene Production from CO2

Author:

Cheng Jian12,Chen Ling3,Xie Xulan1,Feng Kun4,Sun Hao1,Qin Yongze1,Hua Wei1,Zheng Zhangyi1,He Ying1,Pan Weiyi1,Yang Wenjun12,Lyu Fenglei12,Zhong Jun4,Deng Zhao12,Jiao Yan3,Peng Yang12ORCID

Affiliation:

1. Soochow Institute for Energy and Materials Innovations College of Energy Soochow University Suzhou 215006 P. R. China

2. Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215006 P. R. China

3. School of Chemical Engineering The University of Adelaide Adelaide SA 5005 Australia

4. Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Soochow University Suzhou 215123 China

Abstract

AbstractHybrid organic/inorganic composites with the organic phase tailored to modulate local chemical environment at the Cu surface arise as an enchanting category of catalysts for electrocatalytic CO2 reduction reaction (CO2RR). A fundamental understanding on how the organics of different functionality, polarity, and hydrophobicity affect the reaction path is, however, still lacking to guide rational catalyst design. Herein, polypyrrole (PPy) and polyaniline (PANI) manifesting different Brønsted basicity are compared for their regulatory roles on the CO2RR pathways regarding *CO coverage, proton source and interfacial polarity. Concerted efforts from in situ IR, Raman and operando modelling unveil that at the PPy/Cu interface with limited *CO coverage, hydridic *H produced by the Volmer step favors the carbon hydrogenation of *CO to form *CHO through a Tafel process; Whereas at the PANI/Cu interface with concentrated CO2 and high *CO coverage, protonic H+ shuttled through the benzenoid ‐NH‐ protonates the oxygen of *CO, yielding *COH for asymmetric coupling with nearby *CO to form *OCCOH under favored energetics. As a result of the tailored chemical environment, the restructured PANI/Cu composite demonstrates a high partial current density of 0.41 A cm−2 at a maximal Faraday efficiency of 67.5 % for ethylene production, ranking among states of the art.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Jiangsu Province

Six Talent Peaks Project in Jiangsu Province

Australian Research Council

Publisher

Wiley

Subject

General Chemistry,Catalysis

同舟云学术

1.学者识别学者识别

2.学术分析学术分析

3.人才评估人才评估

"同舟云学术"是以全球学者为主线,采集、加工和组织学术论文而形成的新型学术文献查询和分析系统,可以对全球学者进行文献检索和人才价值评估。用户可以通过关注某些学科领域的顶尖人物而持续追踪该领域的学科进展和研究前沿。经过近期的数据扩容,当前同舟云学术共收录了国内外主流学术期刊6万余种,收集的期刊论文及会议论文总量共计约1.5亿篇,并以每天添加12000余篇中外论文的速度递增。我们也可以为用户提供个性化、定制化的学者数据。欢迎来电咨询!咨询电话:010-8811{复制后删除}0370

www.globalauthorid.com

TOP

Copyright © 2019-2024 北京同舟云网络信息技术有限公司
京公网安备11010802033243号  京ICP备18003416号-3