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However, their applications in evaluating 2D van der Waals materials often suffer from substantial interfacial contact resistance at the electrode\/catalyst junction and sluggish catalytic reaction kinetics at the catalyst\/electrolyte interface. Herein, we develop an yttrium\u2010doping strategy for monolayer MoS\n                    <jats:sub>2<\/jats:sub>\n                    (Y\u2010MoS\n                    <jats:sub>2<\/jats:sub>\n                    ) that simultaneously optimizes charge injection across the solid\u2013solid (electrode\/catalyst) interface and hydrogen binding on the basal plane of MoS\n                    <jats:sub>2<\/jats:sub>\n                    . The Y doping downshifts the conduction band minimum of MoS\n                    <jats:sub>2<\/jats:sub>\n                    , lowering the Schottky barrier from 0.47 to 0.23\u00a0eV and enhancing electron injection across the electrode\/catalyst interface. The matching spatial orbital symmetry of Y and Mo 4\n                    <jats:italic>d<\/jats:italic>\n                    <jats:sub>xz\/yz<\/jats:sub>\n                    induces strong\n                    <jats:italic>d\u2010d<\/jats:italic>\n                    electronic coupling, driving the formation of a favorable bridge hydrogen intermediate () with an optimized binding energy of 0.36\u00a0eV for hydrogen evolution reaction (HER) at the catalyst\/electrolyte interface. Benefiting from this synergistic optimization of band alignment and hydrogen binding, Y\u2010MoS\n                    <jats:sub>2<\/jats:sub>\n                    exhibits superior HER performance, delivering an overpotential of 187\u00a0mV at 10\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , competitive with recent 2D MoS\n                    <jats:sub>2<\/jats:sub>\n                    \u2010based electrocatalysts. This work establishes an optimized OCEM platform for decoupled mechanistic analysis and an orbital\u2010level tuning strategy for efficient electrocatalyst design.\n                  <\/jats:p>","DOI":"10.1002\/adma.74673","type":"journal-article","created":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T08:39:37Z","timestamp":1786955977000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Yttrium\u2010Doped MoS\n                    <sub>2<\/sub>\n                    With Optimized Interface Charge Injection and Hydrogen Binding for Efficient Hydrogen Evolution"],"prefix":"10.1002","volume":"38","author":[{"given":"Shen'ao","family":"Xue","sequence":"first","affiliation":[{"name":"School of Physics Central South University  Changsha China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lan","family":"Luo","sequence":"additional","affiliation":[{"name":"School of Physics Central South University  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