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Accelerated Water Oxidation Kinetics Triggered by Supramolecular Porphyrin Nanosheet for Robust Visible-Light-Driven CO2 Reduction
Small ( IF 13.0 ) Pub Date : 2022-11-06 , DOI: 10.1002/smll.202204924 Qian Chen 1 , Yue Zhang 2 , Enming You 1 , Qiaorong Jiang 1 , Xianjie Chen 3 , Yu Wang 1 , Zhijia Song 1 , Kuan Chang 1 , Zhaoxiong Xie 1 , Qin Kuang 1
Small ( IF 13.0 ) Pub Date : 2022-11-06 , DOI: 10.1002/smll.202204924 Qian Chen 1 , Yue Zhang 2 , Enming You 1 , Qiaorong Jiang 1 , Xianjie Chen 3 , Yu Wang 1 , Zhijia Song 1 , Kuan Chang 1 , Zhaoxiong Xie 1 , Qin Kuang 1
Affiliation
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Water oxidation is one of the most challenging steps in CO2 photoreduction, but its influence on CO2 photoreduction is still poorly understood. Herein, the concept of accelerating the water oxidation kinetics to promote the CO2 photoreduction is realized by incorporating supramolecular porphyrin nanosheets (NS) into the C3N4 catalyst. As a prototype, porphyrin-C3N4 based van der Waals heterojunctions with efficient charge separation are elaborately designed, in which the porphyrin and C3N4 NS serve as the water oxidation booster and CO2 reduction center, respectively. Theoretical calculations and relevant experiments demonstrate that the added porphyrin NS reverses the rate-limiting step in the water oxidation while reducing its energy barrier, thus resulting in faster reaction kinetics. Therefore, the optimal sample shows excellent performance in visible-light-driven CO2 reduction with a maximum CO evolution rate of 16.8 µmol g−1 h−1, which is 6.8 times that of the C3N4 NS and reaches the current state of the art for C3N4-based materials in CO2 photoreduction. Overall, this work throws light that accelerating water oxidation kinetics can effectively improve the CO2 photoreduction efficiency.
中文翻译：
超分子卟啉纳米片触发的加速水氧化动力学，用于稳健的可见光驱动 CO2 还原
水氧化是CO 2光还原中最具挑战性的步骤之一，但其对CO 2光还原的影响仍知之甚少。在此，通过将超分子卟啉纳米片 (NS) 结合到 C 3 N 4催化剂中，实现了加速水氧化动力学以促进 CO 2光还原的概念。以卟啉-C 3 N 4为原型，精心设计了具有高效电荷分离的基于卟啉-C 3 N 4的范德华异质结，其中卟啉和C 3 N 4 NS作为水氧化促进剂，CO 2还原中心，分别。理论计算和相关实验表明，添加的卟啉 NS 逆转了水氧化中的限速步骤，同时降低了它的能垒，从而导致更快的反应动力学。因此，最佳样品在可见光驱动的CO 2还原中表现出优异的性能，最大CO释放速率为16.8 µmol g −1 h −1，是C 3 N 4 NS的6.8倍，达到目前的状态CO 2中基于C 3 N 4的材料的最新技术光还原。总的来说，这项工作揭示了加速水氧化动力学可以有效提高 CO 2光还原效率。
更新日期：2022-11-06
中文翻译：
超分子卟啉纳米片触发的加速水氧化动力学，用于稳健的可见光驱动 CO2 还原
水氧化是CO 2光还原中最具挑战性的步骤之一，但其对CO 2光还原的影响仍知之甚少。在此，通过将超分子卟啉纳米片 (NS) 结合到 C 3 N 4催化剂中，实现了加速水氧化动力学以促进 CO 2光还原的概念。以卟啉-C 3 N 4为原型，精心设计了具有高效电荷分离的基于卟啉-C 3 N 4的范德华异质结，其中卟啉和C 3 N 4 NS作为水氧化促进剂，CO 2还原中心，分别。理论计算和相关实验表明，添加的卟啉 NS 逆转了水氧化中的限速步骤，同时降低了它的能垒，从而导致更快的反应动力学。因此，最佳样品在可见光驱动的CO 2还原中表现出优异的性能，最大CO释放速率为16.8 µmol g −1 h −1，是C 3 N 4 NS的6.8倍，达到目前的状态CO 2中基于C 3 N 4的材料的最新技术光还原。总的来说，这项工作揭示了加速水氧化动力学可以有效提高 CO 2光还原效率。
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