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Reversible hydrogen storage of light\u2010weight metal hydrides with high theoretical gravimetric and volumetric hydrogen density is one ideal solution but requires extremely high operating temperature with large energy input. Herein, taking MgH<jats:sub>2<\/jats:sub> as an example, a concept is demonstrated to achieve solar\u2010driven reversible hydrogen storage of metal hydrides via coupling the photothermal effect and catalytic role of Cu nanoparticles uniformly distributed on the surface of MXene nanosheets (Cu@MXene). The photothermal effect of Cu@MXene, coupled with the \u201cheat isolator\u201d role of MgH<jats:sub>2<\/jats:sub> indued by its poor thermal conductivity, effectively elevates the temperature of MgH<jats:sub>2<\/jats:sub> upon solar irradiation. The \u201chydrogen pump\u201d effect of Ti and TiH<jats:italic><jats:sub>x<\/jats:sub><\/jats:italic> species that are in situ formed on the surface of MXene from the reduction of MgH<jats:sub>2<\/jats:sub>, on the other hand, plays a catalytic role in effectively alleviating the kinetic barrier and hence decreasing the operating temperature required for reversible hydrogen adsorption and desorption of MgH<jats:sub>2<\/jats:sub>. Based on the combination of photothermal and catalytic effect of Cu@MXene, a reversible hydrogen storage capacity of 5.9\u00a0wt% is achieved for MgH<jats:sub>2<\/jats:sub> after 30 cycles using solar irradiation as the only energy source.<\/jats:p>","DOI":"10.1002\/adma.202206946","type":"journal-article","created":{"date-parts":[[2022,10,29]],"date-time":"2022-10-29T03:18:45Z","timestamp":1667013525000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":144,"title":["Solar\u2010Driven Reversible Hydrogen Storage"],"prefix":"10.1002","volume":"35","author":[{"given":"Xiaoyue","family":"Zhang","sequence":"first","affiliation":[{"name":"Department of Materials Science Fudan University  Shanghai 200433 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yahui","family":"Sun","sequence":"additional","affiliation":[{"name":"Department of Materials Science Fudan University  Shanghai 200433 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