Huimin Zhang, Ping Song, Xuanhao Mei, Dezheng Zhang, Cong Liu, Mingtao Chu, Teng Zhang, Ce Han, Weilin Xu
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引用次数: 0
Abstract
Developing an efficient and stable bifunctional electrocatalyst for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) in acidic media is of great significance, yet remains challenging. Herein, a bifunctional electrocatalyst supported by carbon cloth, denoted as IrNiOx/WO3, was designed and synthesized through heterostructured coupling of active amorphous IrNiOx with stable crystalline WO3. Benefiting from the pronounced electron interaction stemming from the as-generated numerous heterointerfaces, as-fabricated IrNiOx/WO3 demonstrates a low cell voltage of 1.539 V to achieve 10 mA cm–2 for water splitting with a low Ir loading of 0.8 wt % while maintaining stability over 100 h of continuous electrolysis in 0.5 M H2SO4. Furthermore, through comprehensive structural characterization and theoretical analysis, it was revealed that the Ir sites in the Ir–O–Ni configuration within amorphous IrNiOx serve as the primary active sites for both HER and OER processes. Moreover, the corresponding energy barriers were found to be significantly lowered due to the strong electronic interaction between amorphous IrNiOx and crystalline WO3. This study provides a strategy for designing amorphous–crystalline heterostructured electrocatalysts with ideal interfacial properties for efficient overall water splitting.
开发一种高效、稳定的双功能电催化剂用于酸性介质中析氧反应(OER)和析氢反应(HER)具有重要意义,但仍具有挑战性。本文通过活性非晶IrNiOx与稳定结晶WO3的异质结构耦合,设计并合成了碳布负载的双功能电催化剂IrNiOx/WO3。得益于大量异质界面产生的明显的电子相互作用,制备的IrNiOx/WO3具有1.539 V的低电池电压,在低Ir负载为0.8 wt %的情况下实现10 mA cm-2的水分解,同时在0.5 M H2SO4中连续电解100小时保持稳定性。此外,通过全面的结构表征和理论分析,揭示了非晶IrNiOx中Ir - o - ni结构中的Ir位点是HER和OER过程的主要活性位点。此外,由于非晶IrNiOx和结晶WO3之间存在强电子相互作用,相应的能垒显著降低。该研究为设计具有理想界面性能的非晶异质结构电催化剂提供了一种策略。
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.