Ma Jun, Mao Keke, Low Jingxiang, Wang Zihao, Xi Dawei, Zhang Wenqing, Ju Huanxin, Qi Zeming, Long Ran, Wu Xiaojun, Song Li, Xiong Yujie
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, and CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui, 230026, China.
Institute of Energy, Hefei Comprehensive National Science Center, 350 Shushanhu Rd., Hefei, Anhui, 230031, China.
Angew Chem Int Ed Engl. 2021 Apr 19;60(17):9357-9361. doi: 10.1002/anie.202101701. Epub 2021 Mar 17.
Photoelectrochemical (PEC) conversion of methane (CH ) has been extensively explored for the production of value-added chemicals, yet remains a great challenge in high selectivity toward C products. Herein, we report the optimization of the reactivity of hydroxyl radicals ( OH) on WO via facet tuning to achieve efficient ethylene glycol production from PEC CH conversion. A combination of materials simulation and radicals trapping test provides insight into the reactivity of OH on different facets of WO , showing the highest reactivity of surface-bound OH on {010} facets. As such, the WO with the highest {010} facet ratio exhibits a superior PEC CH conversion efficiency, reaching an ethylene glycol production rate of 0.47 μmol cm h . Based on in situ characterization, the methanol, which could be attacked by reactive OH to form hydroxymethyl radicals, is confirmed to be the main intermediate for the production of ethylene glycol. Our finding is expected to provide new insight for the design of active and selective catalysts toward PEC CH conversion.
甲烷(CH₄)的光电化学(PEC)转化已被广泛研究用于生产高附加值化学品,但在对C产物的高选择性方面仍然是一个巨大挑战。在此,我们报告了通过晶面调控优化WO₃上羟基自由基(·OH)的反应活性,以实现PEC CH₄转化高效生产乙二醇。材料模拟和自由基捕获测试相结合,深入了解了·OH在WO₃不同晶面上的反应活性,表明表面结合的·OH在{010}晶面上具有最高的反应活性。因此,{010}晶面比例最高的WO₃表现出优异的PEC CH₄转化效率,乙二醇产率达到0.47 μmol cm⁻² h⁻¹。基于原位表征,证实可被活性·OH攻击形成羟甲基自由基的甲醇是生产乙二醇的主要中间体。我们的发现有望为设计用于PEC CH₄转化具有活性和选择性的催化剂提供新的见解。