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Rational design of Ruddlesden–Popper perovskite electrocatalyst for oxygen reduction to hydrogen peroxide
SusMat ( IF 18.7 ) Pub Date : 2022-06-04 , DOI: 10.1002/sus2.71
Ning Han 1 , Shihui Feng 2 , Wei Guo 1 , Omar Martinez Mora 1 , Xiaolin Zhao 3 , Wei Zhang 1 , Sijie Xie 1 , Zhenyu Zhou 1 , Zhiwei Liu 4 , Qiong Liu 1 , Kai Wan 1 , Xuan Zhang 1 , Jan Fransaer 1
Affiliation  

Although the oxygen reduction process to hydrogen peroxide (H2O2) is a green option for H2O2 generation, the low activity and selectivity hindered the industry's process. In recent years, the electrochemical synthesis of H2O2 through a 2e transfer method of oxygen reduction reaction (ORR) has piqued the interest of both academics and industry. Metal oxide catalysts have emerged as a novel family of electrochemical catalysts due to their unusual physical, chemical, and electrical characteristics. In this work, we first developed a Ruddlesden–Popper perovskite oxide (Pr2NiO4+δ) as a highly selective and active catalyst for 2e ORR to produce H2O2. Molybdenum was introduced here to adjust the oxidation states of these transition metals with successful substitution into Ni-site to prepare Pr2Ni1-xMoxO4+δ, and the molybdenum substitution improves the H2O2 selectivity during the ORR process, in 0.1 M KOH, from 60% of Pr2NiO4+δ to 79% of Pr2Ni0.8Mo0.2O4+δ at 0.55 V versus RHE. A limiting H2O2 concentration of 0.24 mM for Pr2NiO4+δ and 0.42 mM for Pr2Ni0.8Mo0.2O4+δ was obtained at a constant current of 10 mA/cm2 using a flow-cell reactor using a gas-diffusion electrode.

中文翻译:

Ruddlesden-Popper钙钛矿电催化剂氧还原制过氧化氢的合理设计

虽然氧还原制过氧化氢(H 2 O 2)是H 2 O 2生成的绿色选择,但低活性和选择性阻碍了该行业的进程。近年来,通过氧还原反应(ORR)的2e-转移法电化学合成H 2 O 2引起学术界和工业界的兴趣。金属氧化物催化剂由于其不同寻常的物理、化学和电学特性,已成为一类新型的电化学催化剂。在这项工作中,我们首先开发了 Ruddlesden-Popper 钙钛矿氧化物(Pr 2 NiO 4+δ) 作为 2e ORR 生产 H 2 O 2的高选择性和活性催化剂。这里引入钼来调节这些过渡金属的氧化态,成功取代Ni位,制备Pr 2 Ni 1-x Mo x O 4+δ,钼取代提高了ORR过程中H 2 O 2的选择性,在 0.1 M KOH 中,相对于 RHE,在 0.55 V时从 60% 的 Pr 2 NiO 4+δ到 79% 的 Pr 2 Ni 0.8 Mo 0.2 O 4+δ 。A 限制 H 2 O2浓度为 0.24 mM 的 Pr 2 NiO 4+δ和 0.42 mM 的 Pr 2 Ni 0.8 Mo 0.2 O 4+δ使用使用气体扩散电极的流通池反应器在 10 mA/cm 2的恒定电流下获得.
更新日期:2022-06-04
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