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Herein, this work develops a novel single\u2010atom nanozyme pyroptosis initiator: UK5099 and pyruvate oxidase (POx)\u2010co\u2010loaded Cu\u2010NS single\u2010atom nanozyme (Cu\u2010NS@UK@POx), that not only trigger pyroptosis through cascade biocatalysis to boost the immunogenicity of tumor cells, but also remodel the immunosuppressive TME by targeting pyruvate metabolism. By replacing N with weakly electronegative S, the original spatial symmetry of the Cu\u2010N\n                    <jats:sub>4<\/jats:sub>\n                    electron distribution is changed and the enzyme\u2010catalyzed process is effectively regulated. Compared to spatially symmetric Cu\u2010N\n                    <jats:sub>4<\/jats:sub>\n                    single\u2010atom nanozymes (Cu\u2010N\n                    <jats:sub>4<\/jats:sub>\n                    SA), the S\u2010doped spatially asymmetric single\u2010atom nanozymes (Cu\u2010NS SA) exhibit stronger oxidase activities, including peroxidase (POD), nicotinamide adenine dinucleotide (NADH) oxidase (NOx),\n                    <jats:sc>L<\/jats:sc>\n                    \u2010cysteine oxidase (LCO), and glutathione oxidase (GSHOx), which can cause enough reactive oxygen species (ROS) storms to trigger pyroptosis. Moreover, the synergistic effect of Cu\u2010NS SA, UK5099, and POx can target pyruvate metabolism, which not only improves the immune TME but also increases the degree of pyroptosis. This study provides a two\u2010pronged treatment strategy that can significantly activate antitumor immunotherapy effects via ROS storms, NADH\/glutathione\/\n                    <jats:sc>L<\/jats:sc>\n                    \u2010cysteine consumption, pyruvate oxidation, and lactic acid (LA)\/ATP depletion, triggering pyroptosis and regulating metabolism. This work provides a broad vision for expanding antitumor immunotherapy.\n                  <\/jats:p>","DOI":"10.1002\/adma.202312124","type":"journal-article","created":{"date-parts":[[2024,2,7]],"date-time":"2024-02-07T02:41:06Z","timestamp":1707273666000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":135,"title":["Programmed Targeting Pyruvate Metabolism Therapy Amplified Single\u2010Atom Nanozyme\u2010Activated Pyroptosis for Immunotherapy"],"prefix":"10.1002","volume":"36","author":[{"given":"Rui","family":"Niu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun Jilin 130022 P. R. China"},{"name":"School of Applied Chemistry and Engineering University of Science and Technology of China  Hefei Anhui 230026 P. R. 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