Robust water/seawater-electrolysis hydrogen production at industrial-scale current densities by modulating built-in-outer electric field of catalytic substance

IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
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Abstract

Water/seawater-electrolysis hydrogen generation at industrially relevant rates is economically appealing but remains challenging due to the low activity and long-term stability of catalysts. To address these challenges, by means of the work function theory, we conceive a highly dispersed PdRu five-fold twinned structure supported on amorphous Fe (Cu) oxide (PdRu@MOx, M=Fe or Cu), which has a strong built-in-outer electric field between heterointerfaces and five-fold local symmetry breaking. This results in an optimized interface charge density, improving proton adsorption and kinetics of the hydrogen evolution reaction (HER) at PdRu sites. Consequently, in alkaline electrolysis, PdRu@FeOx requires overpotentials as low as 27 and 110 mV to achieve current densities of 100 and 1000 mA cm−2, respectively, with exceptional catalytic stability for up to 10,000 cycles. Moreover, in alkaline seawater, only a 120 mV overpotential is needed to afford a large current density of 1000 mA cm−2. Notably, the mass activity of PdRu@MOx is 17 and 30 times higher than that of commercial Pt/C catalysts in alkaline water and seawater, respectively. This work will be broadly applicable for designing stable multi-metal-site catalytic substances, opening new possibilities for overall seawater electrolysis at industrial-scale current densities.

通过调节催化物质的内置外电场,以工业规模的电流密度进行稳健的水/海水电解制氢
水/海水电解制氢在经济上很有吸引力,但由于催化剂的低活性和长期稳定性,这种制氢方式仍具有挑战性。为了应对这些挑战,我们通过功函数理论构想了一种高度分散的 PdRu 五倍孪生结构,该结构支撑在无定形的铁(铜)氧化物上(PdRu@MOx,M=铁或铜),在异质界面之间具有很强的内置外电场和五倍局部对称性断裂。这就优化了界面电荷密度,改善了 PdRu 位点的质子吸附和氢进化反应(HER)动力学。因此,在碱性电解中,PdRu@FeOx 需要低至 27 mV 和 110 mV 的过电位,才能分别达到 100 mA cm-2 和 1000 mA cm-2 的电流密度,并且在长达 10,000 次循环中具有优异的催化稳定性。此外,在碱性海水中,只需要 120 mV 的过电位就能获得 1000 mA cm-2 的大电流密度。值得注意的是,在碱性水和海水中,PdRu@MOx 的质量活性分别是商用 Pt/C 催化剂的 17 倍和 30 倍。这项工作将广泛应用于设计稳定的多金属位催化物质,为工业规模电流密度的整体海水电解开辟新的可能性。
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来源期刊
Nano Energy
Nano Energy CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
30.30
自引率
7.40%
发文量
1207
审稿时长
23 days
期刊介绍: Nano Energy is a multidisciplinary, rapid-publication forum of original peer-reviewed contributions on the science and engineering of nanomaterials and nanodevices used in all forms of energy harvesting, conversion, storage, utilization and policy. Through its mixture of articles, reviews, communications, research news, and information on key developments, Nano Energy provides a comprehensive coverage of this exciting and dynamic field which joins nanoscience and nanotechnology with energy science. The journal is relevant to all those who are interested in nanomaterials solutions to the energy problem. Nano Energy publishes original experimental and theoretical research on all aspects of energy-related research which utilizes nanomaterials and nanotechnology. Manuscripts of four types are considered: review articles which inform readers of the latest research and advances in energy science; rapid communications which feature exciting research breakthroughs in the field; full-length articles which report comprehensive research developments; and news and opinions which comment on topical issues or express views on the developments in related fields.
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