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Here, we demonstrate the direct conversion of nitrobenzene and CO\n                    <jats:sub>2<\/jats:sub>\n                    with H\n                    <jats:sub>2<\/jats:sub>\n                    into N\u2010methylaniline in a continuous fixed\u2010bed reactor over a CuZnZrO\n                    <jats:sub>x<\/jats:sub>\n                    catalyst, achieving 99% conversion and 95% selectivity with stable operation exceeding 100\u00a0h. Mechanistic studies identify Cu\u2010ZnO interfaces in the form of Cu\n                    <jats:sup>+<\/jats:sup>\n                    \u2010O\n                    <jats:sub>v<\/jats:sub>\n                    \u2010Zn\n                    <jats:sup>2\u2010\u03b4<\/jats:sup>\n                    serve as active sites for CO\n                    <jats:sub>2<\/jats:sub>\n                    hydrogenation to key intermediate formaldehyde (CH\n                    <jats:sub>2<\/jats:sub>\n                    O*), which couples the CO\n                    <jats:sub>2<\/jats:sub>\n                    hydrogenation and methylation of aniline derived from nitrobenzene hydrogenation in kinetics. The tandem configuration provides intrinsic heat\u2010management benefits, recovering 0.341\u00a0kg of steam (1.5\u00a0MPa, 201\u00b0C) per mole of nitrobenzene\u2014far superior to the methanol consumption characteristic of the conventional three\u2010step route. This work highlights tandem catalysis as an effective reactor\u2010level strategy that bridges atomic\u2010scale active\u2010site engineering with kinetic synergies, advancing continuous\u2010flow CO\n                    <jats:sub>2<\/jats:sub>\n                    valorization toward higher\u2010value amines.\n                  <\/jats:p>","DOI":"10.1002\/anie.3089595","type":"journal-article","created":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T07:22:00Z","timestamp":1784272920000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Engineering Tandem Catalysis for Direct CO\n                    <sub>2<\/sub>\n                    \u2010Enabled N\u2010Methylaniline Synthesis With a Fixed\u2010Bed Flow Reaction Process"],"prefix":"10.1002","volume":"65","author":[{"given":"Jieyun","family":"Zhang","sequence":"first","affiliation":[{"name":"Key Laboratory of Advanced Catalysis, Gansu Province; State Key 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