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Acetic acid (AA), a vital compound in chemical production and materials manufacturing, is conventionally synthesized by starting with coal or methane through multiple steps including high‐temperature transformations. Here we present a new synthesis of AA from ethane through photocatalytic selective oxidation of ethane by H2O2 at 0‐25°C. The catalyst designed for this process comprises g‐C3N4 with anchored Pd1 single‐atom sites. In‐situ studies and computational simulation suggest the immobilized Pd1 atom becomes positively charged under photocatalytic condition. Under photoirradiation, the holes on the Pd1 single‐atom of OH‐Pd1Å/g‐C3N4 serves as a catalytic site for activating a C‐H instead of C‐C of C2H6 with a low activation barrier of 0.14 eV, through a concerted mechanism. Remarkably, the selectivity for synthesizing AA reaches 98.7%, achieved under atmospheric pressure of ethane at 0°C. By integrating photocatalysis with thermal catalysis, we introduce a highly selective, environmentally friendly, energy‐efficient synthetic route for AA, starting from ethane, presenting a promising alternative for AA synthesis. This integration of photocatalysis in low‐temperature oxidation demonstrates a new route of selective oxidation of light alkanes.
Acetic acid (AA), a vital compound in chemical production and materials manufacturing, is conventionally synthesized by starting with coal or methane through multiple steps including high‐temperature transformations. Here we present a new synthesis of AA from ethane through photocatalytic selective oxidation of ethane by H2O2 at 0‐25°C. The catalyst designed for this process comprises g‐C3N4 with anchored Pd1 single‐atom sites. In‐situ studies and computational simulation suggest the immobilized Pd1 atom becomes positively charged under photocatalytic condition. Under photoirradiation, the holes on the Pd1 single‐atom of OH‐Pd1Å/g‐C3N4 serves as a catalytic site for activating a C‐H instead of C‐C of C2H6 with a low activation barrier of 0.14 eV, through a concerted mechanism. Remarkably, the selectivity for synthesizing AA reaches 98.7%, achieved under atmospheric pressure of ethane at 0°C. By integrating photocatalysis with thermal catalysis, we introduce a highly selective, environmentally friendly, energy‐efficient synthetic route for AA, starting from ethane, presenting a promising alternative for AA synthesis. This integration of photocatalysis in low‐temperature oxidation demonstrates a new route of selective oxidation of light alkanes.
Acetic acid (AA), a vital compound in chemical production and materials manufacturing, is conventionally synthesized by starting with coal or methane through multiple steps including high‐temperature transformations. Here we present a new synthesis of AA from ethane through photocatalytic selective oxidation of ethane by H2O2 at 0‐25°C. The catalyst designed for this process comprises g‐C3N4 with anchored Pd1 single‐atom sites. In‐situ studies and computational simulation suggest the immobilized Pd1 atom becomes positively charged under photocatalytic condition. Under photoirradiation, the holes on the Pd1 single‐atom of OH‐Pd1Å/g‐C3N4 serves as a catalytic site for activating a C‐H instead of C‐C of C2H6 with a low activation barrier of 0.14 eV, through a concerted mechanism. Remarkably, the selectivity for synthesizing AA reaches 98.7%, achieved under atmospheric pressure of ethane at 0°C. By integrating photocatalysis with thermal catalysis, we introduce a highly selective, environmentally friendly, energy‐efficient synthetic route for AA, starting from ethane, presenting a promising alternative for AA synthesis. This integration of photocatalysis in low‐temperature oxidation demonstrates a new route of selective oxidation of light alkanes.
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