Gd‐Ni‐Sb‐SnO2 electrocatalysts for active and selective ozone production
Gd‐Ni‐Sb‐SnO2 electrocatalysts for active and selective ozone production
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Gd-Ni-Sb-SnO2 电催化剂用于主动和选择性臭氧生产
DOI：
10.1002/aic.17486
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发表时间：
2021
期刊：
影响因子：
3.7
通讯作者：
Tang, Maureen
中科院分区：
文献类型：
--
作者：
Lansing, James L.;Zhao, Lingyan;Siboonruang, Tana;Attanayake, Nuwan H.;Leo, Angela B.;Fatouros, Peter;Park, So Min;Graham, Kenneth R.;Keith, John A.;Tang, Maureen
溶解臭氧的直接电化学生产可能提供经济的废水处理和卫生或有价值的化学氧化剂。虽然Ni-Sb-SnO 2电催化剂具有用于电化学臭氧生产的最高已知法拉第效率，但活性和选择性尚不足以用于商业实施。这项工作发现，共掺杂Ni和Gd使臭氧选择性比单独Ni增加三倍。这些研究结果是第一次演示的活性掺杂剂比镍在SnO 2。电化学和物理表征表明，臭氧活性的趋势是由化学催化，而不是形态的影响，和导带排列是不是一个催化的描述系统。选择性自由基猝灭实验和热力学能量的量子化学计算表明，形成溶液相中间体的动力学势垒对于理解掺杂剂在电化学臭氧生产中的作用非常重要。
Direct electrochemical production of dissolved ozone could potentially provide economic wastewater treatment and sanitation or a valuable chemical oxidant. Although Ni‐Sb‐SnO2electrocatalysts have the highest known faradaic efficiencies for electrochemical ozone production, the activity and selectivity are not yet sufficient for commercial implementation. This work finds that co‐doping Ni and Gd increases the ozone selectivity by a factor of three over Ni alone. These findings are the first demonstration of an active dopant other than Ni in SnO2. Electrochemical and physical characterization show that trends in ozone activity are caused by chemical catalysis, not morphology effects, and that conduction band alignment is not a catalytic descriptor for the system. Selective radical quenching experiments and quantum chemistry calculations of thermodynamic energies suggest that the kinetic barriers to form solution‐phase intermediates are important for understanding the role of dopants in electrochemical ozone production.