Krishnamoorthy Sathiyan*, Poulami Mukherjee, Koichi Higashimine and Toshiaki Taniike*,
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Among a series of LaCoO<sub>3</sub>–MoS<sub>2</sub> composites synthesized, the composition LCM-100 exhibits the highest electrochemical performance. Unlike physically mixed counterparts with weak interfacial contact and poor charge transport, the hierarchical architecture of LCM-100, featuring edge-exposed MoS<sub>2</sub> nanosheets chemically anchored onto a redox-active, structurally stable LaCoO<sub>3</sub> support, enables strong interfacial coupling and efficient electron transfer. This leads to superior electrocatalytic activity toward both the HER (236 mV) and the OER (1.64 V vs reversible hydrogen electrode, RHE) at 10 mA cm<sup>–2</sup> in alkaline media. In a full water-splitting electrolyzer, LCM-100 coated on a neutral carbon paper substrate initially delivers a cell voltage of 1.70 V<sub>RHE</sub> at 10 mA cm<sup>–2</sup>, which improves to 1.67 V<sub>RHE</sub> after chronopotentiometric activation and exhibits impressive stability at 250 mA cm<sup>–2</sup> for 100 h. 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引用次数: 0
摘要
设计绿色制氢双功能催化剂是实现高效、规模化水电解的关键。虽然双功能电催化剂可以在同一电解质中同时催化析氢反应(HER)和析氧反应(OER),从而降低系统设计的复杂性和运行成本,但将双活性位点整合到一个框架中通常需要在活性和耐久性之间进行权衡。本文报道了一种化学集成的LaCoO3-MoS2 (LCM)复合材料作为碱水分解的无贵金属双功能催化剂。在合成的一系列LaCoO3-MoS2复合材料中,LCM-100的电化学性能最高。LCM-100的层次化结构不同于物理混合的界面接触弱和电荷传输差的对应物,LCM-100的层次化结构将边缘暴露的MoS2纳米片化学固定在氧化还原活性、结构稳定的LaCoO3载体上,实现了强界面耦合和高效电子转移。这导致在碱性介质中对HER (236 mV)和OER (1.64 V vs可逆氢电极,RHE)在10 mA cm-2下具有优异的电催化活性。在全水分解电解槽中,涂覆在中性碳纸衬底上的LCM-100最初在10 mA cm-2下提供1.70 VRHE的电池电压,在时间电位活化后提高到1.67 VRHE,并在250 mA cm-2下表现出令人印象深刻的100小时稳定性。这些发现强调了化学整合在设计无贵金属双功能催化剂方面的有效性。
Durability Meets Performance: A LaCoO3–MoS2 Composite for Electrochemical Overall Water Splitting
Designing bifunctional catalysts for green hydrogen production is the key to realizing efficient and scalable water electrolysis. While bifunctional electrocatalysts can reduce the system design complexity and lower the operational cost by catalyzing both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) within the same electrolyte, incorporating dual active sites into one framework often involves trade-offs between activity and durability. This work reports a chemically integrated LaCoO3–MoS2 (LCM) composite as a noble-metal-free bifunctional catalyst for alkaline water splitting. Among a series of LaCoO3–MoS2 composites synthesized, the composition LCM-100 exhibits the highest electrochemical performance. Unlike physically mixed counterparts with weak interfacial contact and poor charge transport, the hierarchical architecture of LCM-100, featuring edge-exposed MoS2 nanosheets chemically anchored onto a redox-active, structurally stable LaCoO3 support, enables strong interfacial coupling and efficient electron transfer. This leads to superior electrocatalytic activity toward both the HER (236 mV) and the OER (1.64 V vs reversible hydrogen electrode, RHE) at 10 mA cm–2 in alkaline media. In a full water-splitting electrolyzer, LCM-100 coated on a neutral carbon paper substrate initially delivers a cell voltage of 1.70 VRHE at 10 mA cm–2, which improves to 1.67 VRHE after chronopotentiometric activation and exhibits impressive stability at 250 mA cm–2 for 100 h. These findings underscore the effectiveness of chemical integration in designing noble-metal-free bifunctional catalysts for practical water-splitting applications.
期刊介绍:
Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.