Yu Xu, Li Yong, Pei Chengang, Lu Yanhui, Kim Jung Kyu, Park Ho Seok, Pang Huan
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225002, P. R. China.
Department of Chemical Engineering, College of Engineering, Sungkyunkwan University, 2066, Seobu-ro, Jangan-gu, Suwon-si, Gyeonggi-do, 16419, Republic of Korea.
Adv Sci (Weinh). 2024 Jun;11(22):e2310013. doi: 10.1002/advs.202310013. Epub 2024 Mar 29.
The development of a cost-competitive and efficient electrocatalyst is both attractive and challenging for hydrogen production by hydrogen evolution reaction (HER). Herein, a facile glycol reduction method to construct Ru nanoclusters coupled with hierarchical exfoliated-MXene/reduced graphene oxide architectures (Ru-E-MXene/rGA) is reported. The hierarchical structure, formed by the self-assembly of graphene oxides, can effectively prohibit the self-stacking of MXene nanosheets. Meanwhile, the formation of the MXene/rGA interface can strongly trap the Ru ions, resulting in the uniform distribution of Ru nanoclusters within Ru-E-MXene/rGA. The boosted catalytic activity and underlying catalytic mechanism during the HER process are proved by density functional theory. Ru-E-MXene/rGA exhibits overpotentials of 42 and 62 mV at 10 mA cm in alkaline and acidic electrolytes, respectively. The small Tafel slope and charge transfer resistance (R) values elucidate its fast dynamic behavior. The cyclic voltammetry (CV) curves and chronoamperometry test confirm the high stability of Ru-E-MXene/rGA. These results demonstrate that coupling Ru nanoclusters with the MXene/rGA heterostructure represents an efficient strategy for constructing MXene-based catalysts with enhanced HER activity.
开发具有成本竞争力且高效的电催化剂对于通过析氢反应(HER)制氢而言既具有吸引力又具有挑战性。在此,报道了一种简便的乙二醇还原法来构建与分级剥离的MXene/还原氧化石墨烯结构(Ru-E-MXene/rGA)耦合的Ru纳米团簇。由氧化石墨烯自组装形成的分级结构可有效阻止MXene纳米片的自堆叠。同时,MXene/rGA界面的形成可强烈捕获Ru离子,导致Ru纳米团簇在Ru-E-MXene/rGA内均匀分布。密度泛函理论证明了HER过程中催化活性的提高及其潜在的催化机理。Ru-E-MXene/rGA在碱性和酸性电解质中,在10 mA cm时的过电位分别为42和62 mV。较小的塔菲尔斜率和电荷转移电阻(R)值表明其具有快速的动力学行为。循环伏安法(CV)曲线和计时电流法测试证实了Ru-E-MXene/rGA的高稳定性。这些结果表明,将Ru纳米团簇与MXene/rGA异质结构耦合是构建具有增强HER活性的基于MXene的催化剂的有效策略。