华南师范大学兰亚乾团队开发了光、热、电综合能量转换系统用于CO₂和甲醇的光热辅助共电解。相关研究成果于2022年10月13日发表于国际一流学术期刊《德国应用化学》。

为了提高CO₂电还原系统的能量转换效率和氧化还原产物价值，迫切需要设计出功能强大的光热催化剂来实现光热效应辅助耦合催化。

该文中，研究人员制备了一种含共价有机框架的双功能紫精（Ni-2CBpy²⁺-COF），并成功地应用于光热辅助共电解CO₂和甲醇。具体而言，当阳极析氧反应（OER）被甲醇氧化所取代时，Ni-2CBpy²⁺-COF的FE CO（阴极）和FE HCOOH（阳极）在1.9 V时可达到~100%，节省约31.5%的总电耗。如DFT计算和表征所示，Ni-2CBpy²⁺-COF中的环状二喹啉增强了光热效应（ΔT=49.1°C），加快了催化剂和直接物种之间的电荷转移速度，并提高了对所需产品的选择性，具有优异的性能。

附：英文原文

Title: Light, Heat and Electricity Integrated Energy Conversion System: Photothermal-assisted Co-electrolysis of CO2 and Methanol

Author: Yi-Rong Wang, Hui-Min Ding, Sheng-Nan Sun, Jing-Wen Shi, Yi-Lu Yang, Qi Li, Yifa Chen, Shun-Li Li, Ya-Qian Lan

Issue&Volume: 2022-10-13

Abstract: Strategy that can design powerful photothermal-catalysts to achieve photothermal-effect assisted coupling-catalysis is much desired for the improvement of energy conversion efficiency and redox product value in CO  2  electroreduction system. Herein, a kind of bifunctional viologen-containing covalent organic framework (Ni-2CBpy  2+  -COF) has been prepared and successfully applied in photothermal-assisted co-electrolysis of CO  2  and methanol. Specifically, the FE  CO  (cathode) and FE  HCOOH  (anode) for Ni-2CBpy  2+  -COF can reach up to ~100% at 1.9 V with ~31.5% saved overall electricity-consumption when the anodic oxygen evolution reaction (OER) is replaced by methanol oxidation. The superior performance could be attributed to the cyclic diquats in Ni-2CBpy  2+  -COF that enhance the photothermal effect (Δ  T  = 49.1 °C) to accelerate faster charge transfer between catalyst and immediate species as well as higher selectivity towards desired products as revealed by DFT calculations and characterizations.

DOI: 10.1002/anie.202212162

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202212162