Enabling built-in electric fields on rhenium-vacancy-rich heterojunction interfaces of transition-metal dichalcogenides for pH-universal efficient hydrogen and electric energy generation

IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Carbon Energy Pub Date : 2024-04-02 DOI:10.1002/cey2.526
Benzhi Wang, Lixia Wang, Ji Hoon Lee, Tayirjan Taylor Isimjan, Hyung Mo Jeong, Xiulin Yang
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Abstract

Most advanced hydrogen evolution reaction (HER) catalysts show high activity under alkaline conditions. However, the performance deteriorates at a natural and acidic pH, which is often problematic in practical applications. Herein, a rhenium (Re) sulfide–transition-metal dichalcogenide heterojunction catalyst with Re-rich vacancies (NiS2-ReS2-V) has been constructed. The optimized catalyst shows extraordinary electrocatalytic HER performance over a wide range of pH, with ultralow overpotentials of 42, 85, and 122 mV under alkaline, acidic, and neutral conditions, respectively. Moreover, the two-electrode system with NiS2-ReS2-V1 as the cathode provides a voltage of 1.73 V at 500 mA cm−2, superior to industrial systems. Besides, the open-circuit voltage of a single Zn–H2O cell with NiS2-ReS2-V1 as the cathode can reach an impressive 90.9% of the theoretical value, with a maximum power density of up to 31.6 mW cm−2. Moreover, it shows remarkable stability, with sustained discharge for approximately 120 h at 10 mA cm−2, significantly outperforming commercial Pt/C catalysts under the same conditions in all aspects. A series of systematic characterizations and theoretical calculations demonstrate that Re vacancies on the heterojunction interface would generate a stronger built-in electric field, which profoundly affects surface charge distribution and subsequently enhances HER performance.

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在富含铼空位的过渡金属二掺杂化合物异质结界面上实现内置电场,以实现 pH 值通用的高效氢能和电能发电
大多数先进的氢进化反应(HER)催化剂在碱性条件下具有很高的活性。然而,在自然酸性 pH 值条件下,其性能会下降,这在实际应用中往往是个问题。在此,我们构建了一种富含空位(NiS2-ReS2-V)的硫化铼(Re)-过渡金属二卤化物异质结催化剂。优化后的催化剂在广泛的 pH 值范围内显示出非凡的电催化 HER 性能,在碱性、酸性和中性条件下的过电位分别为 42、85 和 122 mV。此外,以 NiS2-ReS2-V1 为阴极的双电极系统在 500 mA cm-2 的条件下可提供 1.73 V 的电压,优于工业系统。此外,以 NiS2-ReS2-V1 为阴极的单个 Zn-H2O 电池的开路电压可达理论值的 90.9%,最大功率密度高达 31.6 mW cm-2。此外,它还表现出了卓越的稳定性,在 10 mA cm-2 下可持续放电约 120 小时,在各方面都明显优于相同条件下的商用 Pt/C 催化剂。一系列系统表征和理论计算表明,异质结界面上的 Re 空位会产生更强的内置电场,从而深刻影响表面电荷分布,进而提高 HER 性能。
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来源期刊
Carbon Energy
Carbon Energy Multiple-
CiteScore
25.70
自引率
10.70%
发文量
116
审稿时长
4 weeks
期刊介绍: Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.
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Issue Information Cover Image, Volume 6, Number 10, October 2024 Back Cover Image, Volume 6, Number 10, October 2024 Interface and doping engineering of V2C-MXene-based electrocatalysts for enhanced electrocatalysis of overall water splitting Issue Information
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