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Herein, by using the tantalum oxide Ta\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>+<\/jats:sup>\n                    as an active cluster, an unprecedented C\n                    <jats:sub>CH4<\/jats:sub>\n                    \u2500C\n                    <jats:sub>CO2<\/jats:sub>\n                    coupling reaction of CH\n                    <jats:sub>4<\/jats:sub>\n                    with CO\n                    <jats:sub>2<\/jats:sub>\n                    to exclusively produce the C\n                    <jats:sub>2<\/jats:sub>\n                    hydrocarbon of C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    has been successfully realized even at room temperature by the state\u2010of\u2010the\u2010art mass spectrometry. The in situ reconstruction from Ta\u2500O\u2500Ta cluster skeleton to tantalum carbide Ta\u2500C\u2500Ta experienced upon the prereaction with CH\n                    <jats:sub>4<\/jats:sub>\n                    is critical to delicately control the sequential elementary reactions targeted for C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    generation. This finding not only leads to a breakthrough in the field of gas\u2010phase and condensed\u2010phase chemistry wherein the C\n                    <jats:sub>2+<\/jats:sub>\n                    oxygenated compounds were the mainstream products for C\n                    <jats:sub>CH4<\/jats:sub>\n                    \u2500C\n                    <jats:sub>CO2<\/jats:sub>\n                    coupling of CH\n                    <jats:sub>4<\/jats:sub>\n                    with CO\n                    <jats:sub>2<\/jats:sub>\n                    , but also explores a new active structure and a novel reaction mechanism beneficial for selective production of C\n                    <jats:sub>2<\/jats:sub>\n                    hydrocarbons from coconversion of CH\n                    <jats:sub>4<\/jats:sub>\n                    and CO\n                    <jats:sub>2<\/jats:sub>\n                    .\n                  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