Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Highly Enhancing CO2 Photoreduction by Metallization of an Imidazole-linked Robust Covalent Organic Framework
Small ( IF 13.0 ) Pub Date : 2023-06-30 , DOI: 10.1002/smll.202303324 Tian-Xiang Luan 1 , Jia-Rui Wang 1 , Keyu Li 1 , Hailian Li 1 , Fuchun Nan 1 , William W Yu 1 , Pei-Zhou Li 1
Small ( IF 13.0 ) Pub Date : 2023-06-30 , DOI: 10.1002/smll.202303324 Tian-Xiang Luan 1 , Jia-Rui Wang 1 , Keyu Li 1 , Hailian Li 1 , Fuchun Nan 1 , William W Yu 1 , Pei-Zhou Li 1
Affiliation
|
Converting CO2 into value-added chemicals to solve the issues caused by carbon emission is promising but challenging. Herein, by embedding metal ions (Co2+, Ni2+, Cu2+, and Zn2+) into an imidazole-linked robust photosensitive covalent organic framework (PyPor-COF), effective photocatalysts for CO2 conversion are rationally designed and constructed. Characterizations display that all of the metallized PyPor-COFs (M-PyPor-COFs) display remarkably high enhancement in their photochemical properties. Photocatalysis reactions reveal that the Co-metallized PyPor-COF (Co-PyPor-COF) achieves a CO production rate as high as up to 9645 µmol g−1 h−1 with a selectivity of 96.7% under light irradiation, which is more than 45 times higher than that of the metal-free PyPor-COF, while Ni-metallized PyPor-COF (Ni-PyPor-COF) can further tandem catalyze the generated CO to CH4 with a production rate of 463.2 µmol g−1 h−1. Experimental analyses and theory calculations reveal that their remarkable performance enhancement on CO2 photoreduction should be attributed to the incorporated metal sites in the COF skeleton, which promotes the adsorption and activation of CO2 and the desorption of generated CO and even reduces the reaction energy barrier for the formation of different intermediates. This work demonstrates that by metallizing photoactive COFs, effective photocatalysts for CO2 conversion can be achieved.
中文翻译：
通过咪唑连接的稳健共价有机框架的金属化高度增强 CO2 光还原
将CO 2转化为增值化学品来解决碳排放带来的问题是有前景的，但也具有挑战性。本文中，通过将金属离子（Co 2+、Ni 2+、Cu 2+和Zn 2+）嵌入咪唑连接的鲁棒光敏共价有机骨架（PyPor-COF）中，合理设计了有效的CO 2转化光催化剂，并建。表征表明，所有金属化 PyPor-COF (M-PyPor-COF) 的光化学性能均显着增强。光催化反应表明，在光照射下，钴金属化PyPor-COF（Co-PyPor-COF）的CO产率高达9645 µmol g −1 h −1，选择性为96.7%，超过比不含金属的PyPor-COF高45倍，而镍金属化PyPor-COF（Ni-PyPor-COF）可以进一步串联催化生成的CO生成CH 4 ，产率为463.2 µmol g -1 h - 1 . 实验分析和理论计算表明，它们对CO 2光还原性能的显着增强应归因于COF骨架中掺入的金属位点，促进了CO 2的吸附和活化以及生成的CO的解吸，甚至降低了反应能垒用于形成不同的中间体。这项工作表明，通过金属化光活性COF，可以实现有效的CO 2转化光催化剂。
更新日期：2023-06-30
中文翻译：
通过咪唑连接的稳健共价有机框架的金属化高度增强 CO2 光还原
将CO 2转化为增值化学品来解决碳排放带来的问题是有前景的，但也具有挑战性。本文中，通过将金属离子（Co 2+、Ni 2+、Cu 2+和Zn 2+）嵌入咪唑连接的鲁棒光敏共价有机骨架（PyPor-COF）中，合理设计了有效的CO 2转化光催化剂，并建。表征表明，所有金属化 PyPor-COF (M-PyPor-COF) 的光化学性能均显着增强。光催化反应表明，在光照射下，钴金属化PyPor-COF（Co-PyPor-COF）的CO产率高达9645 µmol g −1 h −1，选择性为96.7%，超过比不含金属的PyPor-COF高45倍，而镍金属化PyPor-COF（Ni-PyPor-COF）可以进一步串联催化生成的CO生成CH 4 ，产率为463.2 µmol g -1 h - 1 . 实验分析和理论计算表明，它们对CO 2光还原性能的显着增强应归因于COF骨架中掺入的金属位点，促进了CO 2的吸附和活化以及生成的CO的解吸，甚至降低了反应能垒用于形成不同的中间体。这项工作表明，通过金属化光活性COF，可以实现有效的CO 2转化光催化剂。
京公网安备 11010802027423号