Yang Yang, Qian Yumin, Li Haijing, Zhang Zhenhua, Mu Yuewen, Do David, Zhou Bo, Dong Jing, Yan Wenjun, Qin Yong, Fang Li, Feng Renfei, Zhou Jigang, Zhang Peng, Dong Juncai, Yu Guihua, Liu Yuanyue, Zhang Xianming, Fan Xiujun
Institute of Crystalline Materials, Shanxi University, Taiyuan, Shanxi 030006, China.
Institute of Molecular Science, Shanxi University, Taiyuan, Shanxi 030006, China.
Sci Adv. 2020 Jun 5;6(23):eaba6586. doi: 10.1126/sciadv.aba6586. eCollection 2020 Jun.
Single-atom catalysts (SACs) maximize the utility efficiency of metal atoms and offer great potential for hydrogen evolution reaction (HER). Bimetal atom catalysts are an appealing strategy in virtue of the synergistic interaction of neighboring metal atoms, which can further improve the intrinsic HER activity beyond SACs. However, the rational design of these systems remains conceptually challenging and requires in-depth research both experimentally and theoretically. Here, we develop a dual-atom catalyst (DAC) consisting of O-coordinated W-Mo heterodimer embedded in N-doped graphene (WMo-NG), which is synthesized by controllable self-assembly and nitridation processes. In WMo-NG, the O-bridged W-Mo atoms are anchored in NG vacancies through oxygen atoms with W─O─Mo─O─C configuration, resulting in stable and finely distribution. The WMo-NG DAC enables Pt-like activity and ultrahigh stability for HER in pH-universal electrolyte. The electron delocalization of W─O─Mo─O─C configuration provides optimal adsorption strength of H and boosts the HER kinetics, thereby notably promoting the intrinsic activity.
单原子催化剂（SACs）可使金属原子的利用效率最大化，并在析氢反应（HER）方面具有巨大潜力。双金属原子催化剂由于相邻金属原子的协同相互作用而成为一种有吸引力的策略，这可以进一步提高超越单原子催化剂的本征析氢活性。然而，这些体系的合理设计在概念上仍然具有挑战性，需要在实验和理论上进行深入研究。在此，我们开发了一种双原子催化剂（DAC），它由嵌入氮掺杂石墨烯（WMo-NG）中的氧配位W-Mo异二聚体组成，通过可控的自组装和氮化过程合成。在WMo-NG中，O桥连的W-Mo原子通过具有W─O─Mo─O─C构型的氧原子锚定在NG空位中，从而实现稳定且精细的分布。WMo-NG双原子催化剂在pH通用电解质中对析氢反应具有类铂活性和超高稳定性。W─O─Mo─O─C构型的电子离域提供了最佳的H吸附强度并促进了析氢动力学，从而显著提高了本征活性。
