催化作用
电解质
化学
布朗斯特德-洛瑞酸碱理论
氢
无机化学
有机化学
物理化学
电极
作者
Zhigang Chen,Hongyu Wang,Chunyu Zhang,Gou Yinning,Zhongmiao Gong,Yaping Jiang,Hongxiang Zeng,Juan Wang,Fancheng Meng,Yi Cui
出处
期刊:ACS Catalysis
[American Chemical Society]
日期:2025-02-03
卷期号:15 (4): 2885-2895
被引量:11
标识
DOI:10.1021/acscatal.5c00405
摘要
Surface-chemistry tailoring of the catalyst is rather meaningful for activity improvement in the electrocatalytic alkaline hydrogen evolution reaction (HER) for hydrogen production. Herein, we report a mild organic-base-driven intercalation and delamination of bulk MoAlB powder into two-dimensional (2D) nanosheets (MBenes) by taking advantage of the amphoteric nature of interlayer Al atoms. In contrast to the conventional oxygen-containing group (e.g., O and OH) coated 2D MBenes by fully removing the interlayer Al0 atoms in strong alkaline solutions, abundant unusual Al3+ oxyanions (AlOx–) are uniformly decorated on our well-designed organic-alkali-exfoliated 2D MBene surface. Accordingly, the as-obtained Al-rich MBene catalyst exhibits a superior alkaline HER activity with a low overpotential (130 mV) at the typical current density of 10 mA/cm2 and a small Tafel slope (58 mV/dec), nearly 4.6- and 2.2-fold enhancements compared to those of the conventional MBene counterpart, respectively. Comprehensive spectroscopy characterizations and DFT calculations demonstrate that the bridging oxygen atoms in local −Al–O–Mo– structures possess strong Brønsted acid nature with reversible behavior in proton storage and donation, which generally benefits the proton-coupled electron HER process in alkaline electrolyte. Our work may pave an interesting route to design 2D Brønsted acid nanosheets for highly efficient water electrolysis and beyond.
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