دورية أكاديمية

Proton Shuttling by Polyaniline of High Brønsted Basicity for Improved Electrocatalytic Ethylene Production from CO 2

التفاصيل البيبلوغرافية
العنوان: Proton Shuttling by Polyaniline of High Brønsted Basicity for Improved Electrocatalytic Ethylene Production from CO 2
المؤلفون: Cheng, Jian, Chen, Ling, Xie, Xulan, Feng, Kun, Sun, Hao, Qin, Yongze, Hua, Wei, Zheng, Zhangyi, He, Ying, Pan, Weiyi, Yang, Wenjun, Lyu, Fenglei, Zhong, Jun, Deng, Zhao, Jiao, Yan, Peng, Yang
المساهمون: National Natural Science Foundation of China, Natural Science Foundation of Jiangsu Province, Six Talent Peaks Project in Jiangsu Province, Australian Research Council
المصدر: Angewandte Chemie International Edition ; volume 62, issue 44 ; ISSN 1433-7851 1521-3773
بيانات النشر: Wiley
سنة النشر: 2023
المجموعة: Wiley Online Library (Open Access Articles via Crossref)
الوصف: Hybrid 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 CO 2 reduction reaction (CO 2 RR). 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 CO 2 RR 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 CO 2 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.
نوع الوثيقة: article in journal/newspaper
اللغة: English
DOI: 10.1002/anie.202312113
الإتاحة: https://doi.org/10.1002/anie.202312113Test
حقوق: http://onlinelibrary.wiley.com/termsAndConditions#amTest ; http://onlinelibrary.wiley.com/termsAndConditions#vorTest
رقم الانضمام: edsbas.B9547F79
قاعدة البيانات: BASE