Efficient Photoelectrochemical Conversion of Methane into Ethylene Glycol by WO3 Nanobar Arrays

被引：102

作者：

Ma, Jun ^{[1
,2
,3
]}

Mao, Keke ^{[4
]}

Low, Jingxiang ^{[1
,2
]}

Wang, Zihao ^{[1
,2
]}

Xi, Dawei ^{[1
,2
]}

Zhang, Wenqing ^{[1
,2
]}

Ju, Huanxin ^{[1
,2
]}

Qi, Zeming ^{[1
,2
]}

Long, Ran ^{[1
,2
]}

Wu, Xiaojun ^{[1
,2
]}

Song, Li ^{[1
,2
]}

Xiong, Yujie ^{[1
,2
,3
]}

机构：

[1] Univ Sci & Technol China, Collaborat Innovat Ctr Chem Energy Mat iChEM, Hefei Natl Lab Phys Sci Microscale, Sch Chem & Mat Sci,Natl Synchrotron Radiat Lab, Hefei 230026, Anhui, Peoples R China

[2] Univ Sci & Technol China, CAS Ctr Excellence Nanosci, Hefei 230026, Anhui, Peoples R China

[3] Hefei Comprehens Natl Sci Ctr, Inst Energy, 350 Shushanhu Rd, Hefei 230031, Anhui, Peoples R China

[4] Anhui Univ Technol, Sch Energy & Environm Sci, Maanshan 243032, Anhui, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2021年 / 60卷 / 17期

基金：

国家重点研发计划;

关键词：

ethylene glycol; methane; nanostructure; photoelectrochemistry; WO3; PHOTOCATALYTIC OXIDATION; WATER; OXYGEN; CH4; EVOLUTION; DIOXIDE; PLASMON; O-2;

D O I：

10.1002/anie.202101701

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Photoelectrochemical (PEC) conversion of methane (CH4) has been extensively explored for the production of value-added chemicals, yet remains a great challenge in high selectivity toward C2+ products. Herein, we report the optimization of the reactivity of hydroxyl radicals ((OH)-O-.) on WO3 via facet tuning to achieve efficient ethylene glycol production from PEC CH4 conversion. A combination of materials simulation and radicals trapping test provides insight into the reactivity of (OH)-O-. on different facets of WO3, showing the highest reactivity of surface-bound (OH)-O-. on {010} facets. As such, the WO3 with the highest {010} facet ratio exhibits a superior PEC CH4 conversion efficiency, reaching an ethylene glycol production rate of 0.47 mu mol cm(-2) h(-1). Based on in situ characterization, the methanol, which could be attacked by reactive (OH)-O-. 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 CH4 conversion.

引用

页码：9357 / 9361

页数：5

共 40 条

[1] Aqueous Au-Pd colloids catalyze selective CH4 oxidation to CH3OH with O2 under mild conditions [J].