Electrocatalytic N_(2) fixation through N_(2) reduction reaction(NRR)has been regarded as a promising route for sustainable NH_(3) synthesis,while exploring high-performing NRR catalysts is pivotal yet challenging.Her...Electrocatalytic N_(2) fixation through N_(2) reduction reaction(NRR)has been regarded as a promising route for sustainable NH_(3) synthesis,while exploring high-performing NRR catalysts is pivotal yet challenging.Herein,BN quantum dots/Ti_(3)C_(2)T_(x)-MXene(BNQDs/Ti_(3)C_(2)T_(x))heterostructure is demonstrated as an efficient and durable NRR catalyst,exhibiting a high NH_(3) yield of 52.8±3.3μg h^(-1) mg^(-1) with an FE of 19.1±1.6%at0.4 V(vs.RHE),which stand at the high level among all reported BN-and MXene-based NRR catalysts.Theoretical computations reveal that the electronic interactions between BNQDs and Ti_(3)C_(2)T_(x) enrich the electron density of B atoms at the heterointerface and endow them with enhanced electron-donating capability for N_(2) activation and protonation.Meanwhile,the decorated BNQDs can block the active sites of Ti_(3)C_(2)T_(x) for hydrogen evolution,rendering a high N_(2)-to-NH_(3) selectivity.展开更多
基金supported by the National Natural Science Foundation of China(51761024)Natural Science Foundation of Gansu Province(20JR10RA241)+2 种基金Longyuan Youth Innovative and Entrepreneurial Talents Project([2021]17)Central Government Guides Local Science and Technology Development Project(206Z1003G)Key Project of Education Department of Hebei Province(ZD2020339).
文摘Electrocatalytic N_(2) fixation through N_(2) reduction reaction(NRR)has been regarded as a promising route for sustainable NH_(3) synthesis,while exploring high-performing NRR catalysts is pivotal yet challenging.Herein,BN quantum dots/Ti_(3)C_(2)T_(x)-MXene(BNQDs/Ti_(3)C_(2)T_(x))heterostructure is demonstrated as an efficient and durable NRR catalyst,exhibiting a high NH_(3) yield of 52.8±3.3μg h^(-1) mg^(-1) with an FE of 19.1±1.6%at0.4 V(vs.RHE),which stand at the high level among all reported BN-and MXene-based NRR catalysts.Theoretical computations reveal that the electronic interactions between BNQDs and Ti_(3)C_(2)T_(x) enrich the electron density of B atoms at the heterointerface and endow them with enhanced electron-donating capability for N_(2) activation and protonation.Meanwhile,the decorated BNQDs can block the active sites of Ti_(3)C_(2)T_(x) for hydrogen evolution,rendering a high N_(2)-to-NH_(3) selectivity.