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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
ACS Catalysis ( IF 11.3 ) 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
ACS Catalysis ( IF 11.3 ) 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
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.
中文翻译:
2 + 1 > 3: Zn-IrP2/FeP 电极上的三金属位点触发协同效应,激活肼辅助整体水分解的工业级性能
通过一步合成策略构建具有高金属利用率的多功能电极是一项严峻的挑战。本文通过“一步磷酸化”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 计算表明,Ir 和 Fe 分别充当 HER 和 HzOR 位点,促进工业级电流下的整体肼分裂 (OHzS)。特别是 Zn 掺杂剂作为 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 波段中心和吸附中间体能力。正如预期的那样,Zn-IrP2/FeP/IF 只需要 223.0 和 382.0 mV 即可分别驱动 HER 和 HzOR 的 1 A cm–2 的工业级电流密度。值得注意的是,Zn-IrP2/FeP/IF 的 OHzS 电压达到 500 mA cm–2 时,比 OWS 的电压低 1.38 V。总之,三金属位点表现出协同电催化功能,并协同最大限度地提高电催化效率。此外,本研究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和深入研究催化机理的多金属催化剂提供了有价值的思路。
更新日期:2024-11-12
中文翻译:
2 + 1 > 3: Zn-IrP2/FeP 电极上的三金属位点触发协同效应,激活肼辅助整体水分解的工业级性能
通过一步合成策略构建具有高金属利用率的多功能电极是一项严峻的挑战。本文通过“一步磷酸化”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 计算表明,Ir 和 Fe 分别充当 HER 和 HzOR 位点,促进工业级电流下的整体肼分裂 (OHzS)。特别是 Zn 掺杂剂作为 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 波段中心和吸附中间体能力。正如预期的那样,Zn-IrP2/FeP/IF 只需要 223.0 和 382.0 mV 即可分别驱动 HER 和 HzOR 的 1 A cm–2 的工业级电流密度。值得注意的是,Zn-IrP2/FeP/IF 的 OHzS 电压达到 500 mA cm–2 时,比 OWS 的电压低 1.38 V。总之,三金属位点表现出协同电催化功能,并协同最大限度地提高电催化效率。此外,本研究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和深入研究催化机理的多金属催化剂提供了有价值的思路。