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Enabling built-in electric fields on rhenium-vacancy-rich heterojunction interfaces of transition-metal dichalcogenides for pH-universal efficient hydrogen and electric energy generation
Carbon Energy ( IF 20.5 ) Pub Date : 2024-04-02 , DOI: 10.1002/cey2.526
Benzhi Wang 1, 2 , Lixia Wang 1 , Ji Hoon Lee 3 , Tayirjan Taylor Isimjan 4 , Hyung Mo Jeong 2 , Xiulin Yang 1
Affiliation  

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.

中文翻译:

在过渡金属二硫属化物的富含铼空位的异质结界面上实现内置电场,以实现 pH 通用的高效氢气和电能产生

最先进的析氢反应 (HER) 催化剂在碱性条件下表现出高活性。然而,在自然和酸性pH下,其性能会下降,这在实际应用中经常出现问题。在此,构建了一种富含Re空位的硫化铼(Re)-过渡金属二硫属化物异质结催化剂(NiS 2 -ReS 2 -V)。优化后的催化剂在较宽的 pH 范围内表现出非凡的电催化 HER 性能,在碱性、酸性和中性条件下分别具有 42、85 和 122 mV 的超低过电势。此外,以NiS 2 -ReS 2 -V 1作为阴极的双电极系统在500 mA cm -2下提供1.73 V的电压,优于工业系统。此外,以NiS 2 -ReS 2 -V 1为阴极的单个Zn–H 2 O电池的开路电压可以达到理论值的90.9%,最大功率密度高达31.6 mW cm −2。此外,它表现出显着的稳定性,在10 mA cm -2下持续放电约120小时,在所有方面均明显优于相同条件下的商业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建电场,深刻影响表面电荷分布,从而提高HER性能。
更新日期:2024-04-03
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