Direct CO_(2) hydrogenation offers an important strategy for promoting the global carbon balance,but high thermodynamic and kinetic stability of CO_(2) has restricted its applicability to only a handful of industrial ...Direct CO_(2) hydrogenation offers an important strategy for promoting the global carbon balance,but high thermodynamic and kinetic stability of CO_(2) has restricted its applicability to only a handful of industrial sectors.Here,we introduce a proof-of-concept application of the electron-rich Pt surface to promote hydrogen donation for electron-rich MoC particles acting as hydrogen acceptors,thereby constructing hydrogen-rich surface of MoC active centers.Moreover,the formed hydrogen-rich and electronrich surface could greatly decrease reaction activation energy to boost the efficient CO_(2) hydrogenation into formic acid over the MoC centers.The optimized MoC@NC/Pt-0.1(NC:nitrogen-doped carbon)catalyst exhibits a high turnover frequency(TOF)value of 1.2 h^(−1) at a lower temperature of 60℃and a TOF of 24.2 h^(−1) under standard reaction conditions widely used in the literature,exceeding 7 times of MoC@NC catalyst and surpassing the benchmark classical non-noble metal active center-based heterogeneous catalyst.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22071146 and 21931005)the Shanghai Science and Technology Committee(No.23XD1421800)+1 种基金the Shanghai Shuguang Program(No.21SG12)the Shanghai Municipal Science and Technology Major Project.
文摘Direct CO_(2) hydrogenation offers an important strategy for promoting the global carbon balance,but high thermodynamic and kinetic stability of CO_(2) has restricted its applicability to only a handful of industrial sectors.Here,we introduce a proof-of-concept application of the electron-rich Pt surface to promote hydrogen donation for electron-rich MoC particles acting as hydrogen acceptors,thereby constructing hydrogen-rich surface of MoC active centers.Moreover,the formed hydrogen-rich and electronrich surface could greatly decrease reaction activation energy to boost the efficient CO_(2) hydrogenation into formic acid over the MoC centers.The optimized MoC@NC/Pt-0.1(NC:nitrogen-doped carbon)catalyst exhibits a high turnover frequency(TOF)value of 1.2 h^(−1) at a lower temperature of 60℃and a TOF of 24.2 h^(−1) under standard reaction conditions widely used in the literature,exceeding 7 times of MoC@NC catalyst and surpassing the benchmark classical non-noble metal active center-based heterogeneous catalyst.
