2 + 1 > 3: Trimetallic Sites on the Zn-IrP2/FeP Electrode Trigger Synergistic Effect to Activate Industrial-Grade Performance for Hydrazine-Assisted Overall Water Splitting

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-11-12 DOI:10.1021/acscatal.4c05825

Xiaoli Sun, Jie Liu, Yunmei Du, Yanru Liu, Wenna Wang, Dehong Chen, Ruiyong Zhang, Lei Wang

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Abstract

Constructing multifunctional electrodes with high metal utilization by a one-step synthesis strategy is a serious challenge. Herein, Zn-IrP₂/FeP with dual-functional activity induced by trimetallic sites are constructed by the “one-step phosphorization”. Relevant characterizations and DFT calculations reveal that Ir and Fe act as the HER and HzOR sites, respectively, promoting the overall hydrazine splitting (OHzS) at the industrial-level current. Specially the Zn dopant, as an auxiliary active site for Ir–Fe dual-active sites, optimizes the physical structure, electronic configuration, d-band center, and adsorption intermediate capabilities of the Zn-IrP₂/FeP/IF electrode from multiple perspectives. As expected, Zn-IrP₂/FeP/IF only requires 223.0 and 382.0 mV to drive the industrial-grade current density of 1 A cm^–2 for HER and HzOR, respectively. Notably, the voltage of the OHzS for Zn-IrP₂/FeP/IF to reach 500 mA cm^–2 is 1.38 V lower than that of the OWS. In summary, trimetallic sites exhibit synergetic electrocatalytic functions and synergistically maximize electrocatalytic efficiency. Moreover, the multiactive site mechanism of the dopant as an auxiliary active site is innovatively proposed in this work. This presents a valuable idea for designing multimetal catalysts with high metal utilization efficiency and in-depth investigation of catalytic mechanisms.

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2 + 1 > 3：Zn-IrP2/FeP 电极上的三金属位触发协同效应，激活肼辅助整体水分离的工业级性能

通过一步合成策略构建金属利用率高的多功能电极是一项严峻的挑战。本文通过 "一步磷化法 "构建了由三金属位点诱导的具有双功能活性的 Zn-IrP2/FeP 。相关表征和 DFT 计算显示，Ir 和 Fe 分别作为 HER 和 HzOR 位点，在工业级电流下促进了整体肼裂解（OHzS）。特别是 Zn 掺杂作为 Ir-Fe 双活性位点的辅助活性位点，从多个角度优化了 Zn-IrP2/FeP/IF 电极的物理结构、电子构型、d 带中心和吸附中间能力。不出所料，Zn-IrP2/FeP/IF 只需要 223.0 和 382.0 mV 就能分别驱动 HER 和 HzOR 达到 1 A cm-2 的工业级电流密度。值得注意的是，Zn-IrP2/FeP/IF 达到 500 mA cm-2 的 OHzS 电压比 OWS 低 1.38 V。总之，三金属位点具有协同电催化功能，并能协同最大化电催化效率。此外，本研究还创新性地提出了掺杂剂作为辅助活性位点的多活性位点机制。这为设计具有高金属利用效率的多金属催化剂和深入研究催化机理提供了宝贵的思路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

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.