Alaufey Rayan, Keith John A, Tang Maureen
Department of Chemical and Biological Engineering, Drexel University, 3141 Chestnut Street, Philadelphia, Pennsylvania 19104, United States.
Department of Chemical and Petroleum Engineering, University of Pittsburgh, 3700 O'Hara Street, Pittsburgh, Pennsylvania 15261, United States.
J Phys Chem Lett. 2024 Jul 18;15(28):7351-7356. doi: 10.1021/acs.jpclett.4c01150. Epub 2024 Jul 11.
Catalysts for electrochemical ozone production (EOP) face inherent selectivity challenges stemming from thermodynamic constraints. This work establishes a design strategy for minimizing these limitations and inducing EOP activity in tin oxide, which is an intrinsically EOP-inactive material. We propose that selective ozone production using tin oxide catalysts can be broadly achieved by co-doping with two elements: first, n-type dopants to enhance electrical conductivity, and second, transition metal dopants that leach and homogeneously generate essential hydroperoxyl radical intermediates. Synthesizing tantalum, antimony, and tungsten n-type dopants with nickel, cobalt, and iron as transition metal dopants confirms that properly co-doping tin oxide yields EOP-active catalysts. This study offers a robust framework for advancing EOP catalyst design and serves as a case study for the application of fundamental co-catalysis and solid-state physics principles to induce catalytic activity in inert materials.
用于电化学臭氧生成（EOP）的催化剂面临着源于热力学限制的固有选择性挑战。这项工作建立了一种设计策略，以最小化这些限制并在氧化锡中诱导EOP活性，氧化锡是一种本质上无EOP活性的材料。我们提出，使用氧化锡催化剂进行选择性臭氧生成可通过两种元素的共掺杂广泛实现：第一，n型掺杂剂以增强导电性；第二，过渡金属掺杂剂，其浸出并均匀生成必需的氢过氧自由基中间体。将钽、锑和钨n型掺杂剂与镍、钴和铁作为过渡金属掺杂剂进行合成，证实了适当的共掺杂氧化锡可产生EOP活性催化剂。本研究为推进EOP催化剂设计提供了一个强大的框架，并作为将基本共催化和固态物理原理应用于在惰性材料中诱导催化活性的案例研究。
