钌基电催化剂在开发经济实惠的质子交换膜(PEM)电解槽方面展现出巨大的潜力。然而,酸性析氧反应(OER)的恶劣酸性氧化环境,往往会导致Ru活性位点的过度氧化,从而导致严重的活性损失。
该文中,研究人员提出了一种附着在核/壳RuCo/RuCoOx肖特基异质结上的超薄共形耗尽层,它不仅最大限度地提高了活性位点的可用性,还提高了其对酸性OER的耐久性和内在活性。
Operando同步辐射表征结合理论计算表明,肖特基异质结引起的晶格应变和电荷转移,基本上调节了活性位点的电子结构,从而调节了OER途径并抑制了Ru物种的过氧化。
值得注意的是,RuCo/RuCoOx的封闭核/壳结构确保了肖特基异质结,在酸性OER条件下的结构完整性。因此,在0.5 M H2SO4中,核/壳RuCo/RuCoOx肖特基异质结在10 mA cm-2下表现出前所未有的耐久性,高达2500 h,在10 mA cm–2下具有~170 mV的超低过电位。
RuCo/RuCoOx催化剂在质子交换膜(PEM)电解槽中,也表现出优异的耐用性,展示了实际应用的潜力。
附:英文原文
Title: Ultrathin and Conformal Depletion Layer of Core/Shell Heterojunction Enables Efficient and Stable Acidic Water Oxidation
Author: Yang Liu, Yan Huang, Duojie Wu, Haeseong Jang, Jianghua Wu, Huirong Li, Wanxia Li, Feng Zhu, Min Gyu Kim, Donglai Zhou, Xiaoke Xi, Zhanwu Lei, Yuchen Zhang, Yu Deng, Wensheng Yan, M. Danny Gu, Jun Jiang, Shuhong Jiao, Ruiguo Cao
Issue&Volume: September 23, 2024
Abstract: Ru-based electrocatalysts hold great promise for developing affordable proton exchange membrane (PEM) electrolyzers. However, the harsh acidic oxidative environment of the acidic oxygen evolution reaction (OER) often causes undesirable overoxidation of Ru active sites and subsequent serious activity loss. Here, we present an ultrathin and conformal depletion layer attached to the Schottky heterojunction of core/shell RuCo/RuCoOx that not only maximizes the availability of active sites but also improves its durability and intrinsic activity for acidic OER. Operando synchrotron characterizations combined with theoretical calculations elucidate that the lattice strain and charge transfer induced by Schottky heterojunction substantially regulate the electronic structures of active sites, which modulates the OER pathway and suppresses the overoxidation of Ru species. Significantly, the closed core/shell architecture of the RuCo/RuCoOx ensures the structure integrity of the Schottky heterojunction under acidic OER conditions. As a result, the core/shell RuCo/RuCoOx Schottky heterojunction exhibits an unprecedented durability up to 250 0 h at 10 mA cm–2 with an ultralow overpotential of ~170 mV at 10 mA cm–2 in 0.5 M H2SO4. The RuCo/RuCoOx catalyst also demonstrates superior durability in a proton exchange membrane (PEM) electrolyzer, showcasing the potential for practical applications.
DOI: 10.1021/jacs.4c07995
Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c07995
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000