Design of the catalyst for efficient water dissociation and hydrogen recombination is paramount in enhancement of the alkaline water electrolysis kinetics.Herein,we reported a delicate hierarchical(VO)_(2) P_(2)O_(7)-...Design of the catalyst for efficient water dissociation and hydrogen recombination is paramount in enhancement of the alkaline water electrolysis kinetics.Herein,we reported a delicate hierarchical(VO)_(2) P_(2)O_(7)-Ni_(2) P@NF(VPO-Ni_(2) P@NF)hybrid catalyst that operated efficiently in alkaline media.The VPO and Ni_(2) P respectively act as the water dissociation promoter and the hydrogen recombination center,which synergistically propel water adsorption/dissociation and H intermediates recombination.The resulting synergistic interfaces between VPO and Ni_(2) P are verified to afford the catalyst an outstanding performance for hydrogen evolution reaction in alkaline media with an overpotential of 154 mV at 10 mA cm^(-2),Tafel slope of 65 mV dec^(-1),and remarkable durability.Furthermore,the catalyst presents the potential for overall water splitting.This work may shed fresh light on the high-performance electrocatalyst design and the application of VPO on water electrolysis.展开更多
通过建立钒磷氧催化剂活性晶相(VO)_(2)P_(2)O_(7)团簇的结构模型,对反应物NO、NH_(3)在V2P2O15H12团簇表面的吸附特性进行了密度泛函(DFT)模拟计算。结果表明,NO分子在团簇表面O1位点的吸附能为-36.62 k J/mol,为物理吸附;NO分子在O_(2...通过建立钒磷氧催化剂活性晶相(VO)_(2)P_(2)O_(7)团簇的结构模型,对反应物NO、NH_(3)在V2P2O15H12团簇表面的吸附特性进行了密度泛函(DFT)模拟计算。结果表明,NO分子在团簇表面O1位点的吸附能为-36.62 k J/mol,为物理吸附;NO分子在O_(2)、O_(3)位点的吸附能分别为-74.95 k J/mol和-47.31 k J/mol,为化学吸附。NH_(3)能够在团簇表面的L酸和B酸形成稳定的化学吸附。结合吸附结果对脱硝反应机理进行了推导,(VO)_(2)P_(2)O_(7)表面的脱硝反应同时遵循L-H和E-R机制。展开更多
基金supported by the National Natural Science Foundation of China(No.51902232)。
文摘Design of the catalyst for efficient water dissociation and hydrogen recombination is paramount in enhancement of the alkaline water electrolysis kinetics.Herein,we reported a delicate hierarchical(VO)_(2) P_(2)O_(7)-Ni_(2) P@NF(VPO-Ni_(2) P@NF)hybrid catalyst that operated efficiently in alkaline media.The VPO and Ni_(2) P respectively act as the water dissociation promoter and the hydrogen recombination center,which synergistically propel water adsorption/dissociation and H intermediates recombination.The resulting synergistic interfaces between VPO and Ni_(2) P are verified to afford the catalyst an outstanding performance for hydrogen evolution reaction in alkaline media with an overpotential of 154 mV at 10 mA cm^(-2),Tafel slope of 65 mV dec^(-1),and remarkable durability.Furthermore,the catalyst presents the potential for overall water splitting.This work may shed fresh light on the high-performance electrocatalyst design and the application of VPO on water electrolysis.
文摘通过建立钒磷氧催化剂活性晶相(VO)_(2)P_(2)O_(7)团簇的结构模型,对反应物NO、NH_(3)在V2P2O15H12团簇表面的吸附特性进行了密度泛函(DFT)模拟计算。结果表明,NO分子在团簇表面O1位点的吸附能为-36.62 k J/mol,为物理吸附;NO分子在O_(2)、O_(3)位点的吸附能分别为-74.95 k J/mol和-47.31 k J/mol,为化学吸附。NH_(3)能够在团簇表面的L酸和B酸形成稳定的化学吸附。结合吸附结果对脱硝反应机理进行了推导,(VO)_(2)P_(2)O_(7)表面的脱硝反应同时遵循L-H和E-R机制。
