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Herein, a series of metal\u2010organic frameworks (MOFs), namely UiO\u201066(n) with exposed \u2500COOH groups, are fabricated by employing both terephthalic acid and 1,2,4\u2010benzenetricarboxylic acid linkers. Following by introducing Cu nanoparticles, Cu@UiO\u201066(n) are synthesized. By regulating the amount of exposed \u2500COOH groups on the MOF pore wall, the interaction between Cu and the MOF support is regulated. This \u2500COOH microenvironment regulates the overall Cu\n                    <jats:sup>0<\/jats:sup>\n                    \/Cu\n                    <jats:sup>+<\/jats:sup>\n                    ratio in the supported Cu species, thereby tuning the Cu\n                    <jats:sup>0<\/jats:sup>\n                    \/Cu\n                    <jats:sup>+<\/jats:sup>\n                    interfacial descriptor, which is closely associated with the CO\n                    <jats:sub>2<\/jats:sub>\n                    hydrogenation performance. The Cu@UiO\u201066(25) featuring the longest Cu\n                    <jats:sup>0<\/jats:sup>\n                    \/Cu\n                    <jats:sup>+<\/jats:sup>\n                    interface achieves a methanol space\u2010time yield of 694\u00a0g kg\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    and methanol selectivity of 92.8% at 250 \u00b0C and 4\u00a0MPa, far surpassing other counterparts. This work provides a deep understanding of the synergistic effect between Cu\n                    <jats:sup>0<\/jats:sup>\n                    and Cu\n                    <jats:sup>+<\/jats:sup>\n                    species in catalytic CO\n                    <jats:sub>2<\/jats:sub>\n                    hydrogenation.\n                  <\/jats:p>","DOI":"10.1002\/anie.4716315","type":"journal-article","created":{"date-parts":[[2026,7,6]],"date-time":"2026-07-06T14:29:11Z","timestamp":1783348151000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Incorporation of Engineered Cu\n                    <sup>0<\/sup>\n                    \/Cu\n                    <sup>+<\/sup>\n                    Interfaces in Metal\u2010Organic Frameworks for Boosting CO\n                    <sub>2<\/sub>\n                    Hydrogenation to Methanol"],"prefix":"10.1002","volume":"65","author":[{"given":"Xiao\u2010Mei","family":"Lei","sequence":"first","affiliation":[{"name":"Hefei National Research Center for Physical Sciences At the Microscale Department of Chemistry University of Science and Technology of China  Hefei Anhui P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiajia","family":"Huang","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences At the Microscale Department of Chemistry University of Science and Technology of China  Hefei Anhui P. R. China"},{"name":"Fujian Provincial Key Laboratory of Soil Environmental Health and Regulation College of Resources and Environment Fujian Agriculture and Forestry University  Fuzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li\u2010Li","family":"Ling","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences At the Microscale Department of Chemistry University of Science and Technology of China  Hefei Anhui P. R. China"},{"name":"Institute of Future Technologies Deep Space Exploration Laboratory  Hefei Anhui P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiayi","family":"Xu","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences At the Microscale Department of Chemistry University of Science and Technology of China  Hefei Anhui P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming\u2010Liang","family":"Gao","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences At the Microscale Department of Chemistry University of Science and Technology of China  Hefei Anhui P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4060-8830","authenticated-orcid":false,"given":"Jingyao","family":"Liu","sequence":"additional","affiliation":[{"name":"Institute of Theoretical Chemistry College of Chemistry Jilin University  Changchun Jilin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hai\u2010Long","family":"Jiang","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences At the Microscale Department of Chemistry University of Science and Technology of China  Hefei Anhui P. R. China"},{"name":"Department of Radiation Oncology Division of Life Sciences and Medicine The First Affiliated Hospital of USTC University of Science and Technology of China  Hefei Anhui P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,7,6]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.7b00435"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8CS00829A"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.adn9388"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200462121"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.5b00007"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.3c00551"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.9b00723"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/s44160\u2010025\u201000747\u20101"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202311241"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1253057"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2020.08.026"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1219831"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.1701290"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1093\/nsr\/nwae114"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010020\u201015445\u2010z"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1093\/nsr\/nwad043"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aaf0718"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adr3332"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010021\u201000684\u20100"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010022\u201000840\u20100"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010023\u201043679\u20100"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.xinn.2023.100445"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja3034153"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c10685"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.0c04371"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jechem.2022.10.034"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.6b05791"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aal3573"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202500118"},{"key":"e_1_2_8_31_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010024\u201001236\u2010y"},{"key":"e_1_2_8_32_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202420126"},{"key":"e_1_2_8_33_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1230444"},{"key":"e_1_2_8_34_1","doi-asserted-by":"publisher","DOI":"10.1039\/C4CS90059F"},{"key":"e_1_2_8_35_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201705189"},{"key":"e_1_2_8_36_1","doi-asserted-by":"publisher","DOI":"10.1016\/S1872\u20102067(22)64193\u20107"},{"key":"e_1_2_8_37_1","doi-asserted-by":"publisher","DOI":"10.1039\/C6CS00724D"},{"key":"e_1_2_8_38_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2020.11.023"},{"key":"e_1_2_8_39_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201800702"},{"key":"e_1_2_8_40_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.7b00058"},{"key":"e_1_2_8_41_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202415155"},{"key":"e_1_2_8_42_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202404931"},{"key":"e_1_2_8_43_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202116396"},{"key":"e_1_2_8_44_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202308089"},{"key":"e_1_2_8_45_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcat.2022.06.026"},{"key":"e_1_2_8_46_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.3c03431"},{"key":"e_1_2_8_47_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2022.122329"},{"key":"e_1_2_8_48_1","doi-asserted-by":"publisher","DOI":"10.1039\/D2SC03723H"},{"key":"e_1_2_8_49_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.4c04577"},{"key":"e_1_2_8_50_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.4c06447"},{"key":"e_1_2_8_51_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.1c03283"},{"key":"e_1_2_8_52_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010019\u20100226\u20106"},{"key":"e_1_2_8_53_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.0c02909"},{"key":"e_1_2_8_54_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.1c04504"},{"key":"e_1_2_8_55_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010024\u201046513\u20103"},{"key":"e_1_2_8_56_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.20181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