Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optim...Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional(3D)hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07°and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm^(-2).The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm^(-2),which is approximately 209 mV lower than water electrolysis.展开更多
Correction for‘An electrodeposited superaerophobic nickel catalyst on pencil-drawn paper:a novel approach for highly efficient and stable hydrogen evolution’by Qian Sun et al.,Inorg.Chem.Front.,2024,https://doi.org/...Correction for‘An electrodeposited superaerophobic nickel catalyst on pencil-drawn paper:a novel approach for highly efficient and stable hydrogen evolution’by Qian Sun et al.,Inorg.Chem.Front.,2024,https://doi.org/10.1039/D4QI00101J.展开更多
Two-dimensional layered transition metal carbides(MXenes),have huge potential advantage for applications in hydrogen evolution reaction(HER).However,the hindered hydrogen evolution at large current densities and the i...Two-dimensional layered transition metal carbides(MXenes),have huge potential advantage for applications in hydrogen evolution reaction(HER).However,the hindered hydrogen evolution at large current densities and the instability of MXenes during HER remains major challenges.Herein,we report the MoS_(2)/Mo_(2)CT_(x) nanoarray with aerophobic structure via molten salt synthesis.In situ vertical distribution of MoS_(2)nanoarray on the surface of Mo_(2)CT_(x) accelerates hydrogen gas release from the electrode,exhibiting significantly enhanced catalytic activity and stability to bare MoS_(2)and Mo_(2)CT_(x).The MoS_(2)/Mo_(2)CT_(x) nanoarray possesses excellent stability at100 mA/cm^(2)for 100 h with only 3%overpotential increase.Our work provides guidance for developing high-stability MXene-based catalysts by virtue of in situ bonding between nanoarray and MXene.展开更多
基金financially supported by the National Key R&D Program of China(2022YFA1503003)the National Natural Science Foundation of China(91961111,22271081)+3 种基金the Natural Science Foundation of Heilongjiang Province(ZD2021B003)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(UNPYSCT-2020004)The Basic Research Fund of Heilongjiang University in Heilongjiang Province(2021-KYYWF-0039)the Heilongjiang University Excellent Youth Foundation。
文摘Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional(3D)hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07°and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm^(-2).The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm^(-2),which is approximately 209 mV lower than water electrolysis.
文摘Correction for‘An electrodeposited superaerophobic nickel catalyst on pencil-drawn paper:a novel approach for highly efficient and stable hydrogen evolution’by Qian Sun et al.,Inorg.Chem.Front.,2024,https://doi.org/10.1039/D4QI00101J.
基金supported by the National Science Fund for Distinguished Young Scholars(No.21925603)the National Natural Science Foundation of China(No.22176190)the Ningbo Toptalent Team Program(No.2018A610005).
文摘Two-dimensional layered transition metal carbides(MXenes),have huge potential advantage for applications in hydrogen evolution reaction(HER).However,the hindered hydrogen evolution at large current densities and the instability of MXenes during HER remains major challenges.Herein,we report the MoS_(2)/Mo_(2)CT_(x) nanoarray with aerophobic structure via molten salt synthesis.In situ vertical distribution of MoS_(2)nanoarray on the surface of Mo_(2)CT_(x) accelerates hydrogen gas release from the electrode,exhibiting significantly enhanced catalytic activity and stability to bare MoS_(2)and Mo_(2)CT_(x).The MoS_(2)/Mo_(2)CT_(x) nanoarray possesses excellent stability at100 mA/cm^(2)for 100 h with only 3%overpotential increase.Our work provides guidance for developing high-stability MXene-based catalysts by virtue of in situ bonding between nanoarray and MXene.
