التفاصيل البيبلوغرافية
| العنوان: |
Pulse Electrolysis Turns on CO 2 Methanation through N‐Confused Cupric Porphyrin |
| المؤلفون: |
Hua, Wei, Liu, Tingting, Zheng, Zhangyi, Yuan, Huihong, Xiao, Long, Feng, Kun, Hui, Jingshu, Deng, Zhao, Ma, Mutian, Cheng, Jian, Song, Daqi, Lyu, Fenglei, Zhong, Jun, Peng, Yang |
| المساهمون: |
National Natural Science Foundation of China, Natural Science Foundation of Jiangsu Province, Suzhou Municipal Science and Technology Bureau |
| المصدر: |
Angewandte Chemie International Edition ; volume 63, issue 12 ; ISSN 1433-7851 1521-3773 |
| بيانات النشر: |
Wiley |
| سنة النشر: |
2024 |
| المجموعة: |
Wiley Online Library (Open Access Articles via Crossref) |
| الوصف: |
Breaking the D 4h symmetry in the square‐planar M−N 4 configuration of macrocycle molecular catalysts has witnessed enhanced electrocatalytic activity, but at the expense of electrochemical stability. Herein, we hypothesize that the lability of the active Cu−N 3 motifs in the N‐confused copper (II) tetraphenylporphyrin (CuNCP) could be overcome by applying pulsed potential electrolysis (PPE) during electrocatalytic carbon dioxide reduction. We find that applying PPE can indeed enhance the CH 4 selectivity on CuNCP by 3 folds to reach the partial current density of 170 mA cm −2 at >60 % Faradaic efficiency (FE) in flow cell. However, combined ex situ X‐ray diffraction (XRD), transmission electron microscope (TEM), and in situ X‐ray absorption spectroscopy (XAS), infrared (IR), Raman, scanning electrochemical microscopy (SECM) characterizations reveal that, in a prolonged time scale, the decomplexation of CuNCP is unavoidable, and the promoted water dissociation under high anodic bias with lowered pH and enriched protons facilitates successive hydrogenation of *CO on the irreversibly reduced Cu nanoparticles, leading to the improved CH 4 selectivity. As a key note, this study signifies the adaption of electrolytic protocol to the catalyst structure for tailoring local chemical environment towards efficient CO 2 reduction. |
| نوع الوثيقة: |
article in journal/newspaper |
| اللغة: |
English |
| DOI: |
10.1002/anie.202315922 |
| الإتاحة: |
https://doi.org/10.1002/anie.202315922Test |
| حقوق: |
http://onlinelibrary.wiley.com/termsAndConditions#vorTest |
| رقم الانضمام: |
edsbas.76BA752D |
| قاعدة البيانات: |
BASE |
