文献类型：期刊文献

英文题名：An Atomically Dispersed Pd Sub-Metallene: Intermediate State of Single Atoms and Metal Bonds

作者：Chu, Tianshu[1,2];Tian, Pengfei[1,2];Wang, Guiying[1,2];Jia, Yanyan[3,4];Dai, Sheng[3,4];Rong, Chao[1,2];Zhang, Bowei[1,2];Xuan, Fu-Zhen[1]

机构：[1]East China Univ Sci & Technol, Sch Mech & Power Engn, Shanghai Key Lab Intelligent Sensing & Detect Tech, Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Pressure Syst & Safety, Minist Educ, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr Fronti, Joint Int Res Lab Precis Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2025

卷号：37

期号：29

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20251918380987);WOS:【SCI-EXPANDED(收录号:WOS:001481735500001)】；

基金：This work was supported by the National Natural Science Foundation of China (No. 52422505, 12274124), the Innovative Research Group Project of the National Natural Science Foundation of China (No. 52321002), the Shanghai Pilot Program for Basic Research (No. 22TQ1400100-6), the Science and Technology Commission of Shanghai Municipality (22ZR1415700), the Shanghai Rising-star Program (20QA1402400), and the Fundamental Research Funds for the Central Universities. Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center at the East China University of Science and Technology.

语种：英文

外文关键词：hydrogen; metal bonds; metallene; sensing; single atom catalysts

摘要：Despite the metal coordination and single-atom catalyst (SAC) have been extensively investigated in surface science over the past decade, their overall activity in involving multi-step reactions remains unsatisfactory owing to the metal bond and single atom being irreconcilable. Here, a stable atomically dispersed Pd sub-metallene (Pd ADSM) layer supported on the 2D MXene (Mo2TiC2) is reported, which combines the advantages of 2D structures, single atoms, and metal bonds. Pd ADSM shows covalent structures along the z-coordination and highly coordinated metal bonds in the 2D direction. During the alkaline hydrogen evolution reaction (HER), Pd ADSM shows 7- and 112-times higher mass activity than the SAC (Pd SAC) and commercial Pt/C at the overpotential of -108 mV, respectively. Operando characterizations and theoretical calculations reveal that the Pd & horbar;Pd interface not only makes the adsorbed water form a flexible hydrogen-bonded skeleton closer to the catalytic center but also reduces the energy barrier for the HER rate-determining step. Moreover, the moderate adsorption energy of Pd & horbar;Pd bonds in ADSM can rapidly activate, dissociate, and desorb hydrogen molecules at room temperature, resulting in record-high hydrogen sensing performances (Response time, Recovery time, and Sensitivity for 100 ppm H2 are 4.8, 1.6 s, and 43.5%, respectively).