The development of cost-effective and highly stable electrocatalysts for oxygen evolution reactions holds paramount importance in practical hydrogen production.Herein,we present a novel self-supported electrode compri...The development of cost-effective and highly stable electrocatalysts for oxygen evolution reactions holds paramount importance in practical hydrogen production.Herein,we present a novel self-supported electrode comprising Ce-doped Ni-Fe-Se nanosheets grown on carbon cloth(Ni-Fe-Ce-Se/CC).This electrode was synthesized through a selenylation process,utilizing Ni-Fe-Ce-layered double hydroxide/carbon cloth(Ni-Fe-Ce LDH/CC)as the precursor.Notably,Ni-Fe-Ce-Se/CC electrode demonstrates remarkable performance,requiring a low overpotential of 300 mV to attain a current density of 100 mA·cm^(-2)under harsh alkaline conditions.Furthermore,the electrode exhibits exceptional stability during continuous operation for 100 h.Insight into the underlying mechanisms was gained through a combination of experimental results and density functional theory calculations.Our findings reveal that Ce doping induces crystal structure deformation in Ni-Fe-Se and enhances electron enrichment around Ni atoms.This structural modification optimizes the adsorption energy of oxygen-based intermediates on the Ni-Fe-Se surface.This work offers a valuable strategy for regulating the electron transfer and adsorption capabilities of transition metal selenide electrocatalysts through RE atoms doping,opening new avenues for enhanced electrocatalytic performance.展开更多
Balancing electron transfer and intermediate adsorption ability of bifunctional catalysts via tailoring electronic structures is crucial for green hydrogen production,while it still remains challenging due to lacking ...Balancing electron transfer and intermediate adsorption ability of bifunctional catalysts via tailoring electronic structures is crucial for green hydrogen production,while it still remains challenging due to lacking efficient strategies.Herein,one efficient and universal strategy is developed to greatly regulate electronic structures of the metallic Ni-Fe-P catalysts via in-situ introducing the rare earth(RE)atoms(Ni-Fe-RE-P,RE=La,Ce,Pr,and Nd).Accordingly,the as-prepared optimal Ni-Fe-Ce-P/CC self-supported bifunctional electrodes exhibited superior electrocatalytic activity and excellent stability with the low overpotentials of 247 and 331 mV at 100 mA cm^(-2) for HER and OER,respectively.In the assembled electrolyzer,the Ni-Fe-Ce-P/CC as bifunctional electrodes displayed low operation potential of 1.49 V to achieve a current density of 10 mA cm^(-2),and the catalytic performance can be maintained for 100 h.Experimental results combined with density functional theory(DFT)calculation reveal that Ce doping leads to electron decentralization and crystal structure distortion,which can tailor the band structures and d-band center of Ni-Fe-P,further increasing conductivity and optimizing intermediate adsorption energy.Our work not only proposes a valuable strategy to regulate the electron transfer and intermediate adsorption of electrocatalysts via RE atoms doping,but also provides a deep under-standing of regulation mechanism of metallic electrocatalysts for enhanced water splitting.展开更多
Enhancing the activity of photocatalysts is a critical challenge for improving the photocatalytic degradation of contaminated wastewater.Here,a novel Ce single-atom-doped titanate nanotube photocatalyst(CeH_(2)Ti_(2)O...Enhancing the activity of photocatalysts is a critical challenge for improving the photocatalytic degradation of contaminated wastewater.Here,a novel Ce single-atom-doped titanate nanotube photocatalyst(CeH_(2)Ti_(2)O_(5)·H_(2)O)was successfully synthesized using a onepot solvothermal method.Degradation experiments revealed that the optimal Ce doping ratio was 1.0%.The ultraviolet-visible diffuse reflectance spectroscopy results showed that the bandgap of the Ce-doped sample decreased from 3.02 to 2.87 eV,enhancing the absorption in the visible spectral range.At the same time,the BrunauerEmmett-Teller specific surface area increased from 63.68 to 88.95 m^(2)g^(-1).The 1.0%Ce-H_(2)Ti_(2)O_(5)·H_(2)O(HTC_(1))could degrade 99.04%of 100 mg L-1rhodamine B(RhB)after 40 min of visible-light irradiation.The degradation efficiency decreased by only 21.24%after five cycles.The results of free-radical quenching and electron spin resonance spectroscopy analyses indicated that HTC_(1)achieved efficient degradation of RhB through a direct hole oxidation mechanism.Compared with pure protonated titanate nanotubes(H_(2)Ti_(2)O_(5)·H_(2)O),HTC_(1)had a higher specific surface area,more electron traps,narrower bandgap,longer hole lifetime,and suppressed photogenerated charge recombination rate owing to the Ce single-atom doping.展开更多
基金supported by the National Key Technology R&D Program of China(Nos.2021YFB3500801,2022YFB3504302 and 2022YFC3901503)the Natural Science Foundation and Overseas Talent Projects of Jiangxi Province(Nos.0232BAB214025 and 20232BCJ25044)the Double Thousand Plan of Jiangxi Province(No.jxsq2023201002).
文摘The development of cost-effective and highly stable electrocatalysts for oxygen evolution reactions holds paramount importance in practical hydrogen production.Herein,we present a novel self-supported electrode comprising Ce-doped Ni-Fe-Se nanosheets grown on carbon cloth(Ni-Fe-Ce-Se/CC).This electrode was synthesized through a selenylation process,utilizing Ni-Fe-Ce-layered double hydroxide/carbon cloth(Ni-Fe-Ce LDH/CC)as the precursor.Notably,Ni-Fe-Ce-Se/CC electrode demonstrates remarkable performance,requiring a low overpotential of 300 mV to attain a current density of 100 mA·cm^(-2)under harsh alkaline conditions.Furthermore,the electrode exhibits exceptional stability during continuous operation for 100 h.Insight into the underlying mechanisms was gained through a combination of experimental results and density functional theory calculations.Our findings reveal that Ce doping induces crystal structure deformation in Ni-Fe-Se and enhances electron enrichment around Ni atoms.This structural modification optimizes the adsorption energy of oxygen-based intermediates on the Ni-Fe-Se surface.This work offers a valuable strategy for regulating the electron transfer and adsorption capabilities of transition metal selenide electrocatalysts through RE atoms doping,opening new avenues for enhanced electrocatalytic performance.
基金support from the National Key Technology R&D Program of China(2021YFB3500801,2022YFC3901503,2022YFB3504302)the Natural Science Foundation and Overseas Talent Projects of Jiangxi Province(20232BAB214025,20232BCJ25044).
文摘Balancing electron transfer and intermediate adsorption ability of bifunctional catalysts via tailoring electronic structures is crucial for green hydrogen production,while it still remains challenging due to lacking efficient strategies.Herein,one efficient and universal strategy is developed to greatly regulate electronic structures of the metallic Ni-Fe-P catalysts via in-situ introducing the rare earth(RE)atoms(Ni-Fe-RE-P,RE=La,Ce,Pr,and Nd).Accordingly,the as-prepared optimal Ni-Fe-Ce-P/CC self-supported bifunctional electrodes exhibited superior electrocatalytic activity and excellent stability with the low overpotentials of 247 and 331 mV at 100 mA cm^(-2) for HER and OER,respectively.In the assembled electrolyzer,the Ni-Fe-Ce-P/CC as bifunctional electrodes displayed low operation potential of 1.49 V to achieve a current density of 10 mA cm^(-2),and the catalytic performance can be maintained for 100 h.Experimental results combined with density functional theory(DFT)calculation reveal that Ce doping leads to electron decentralization and crystal structure distortion,which can tailor the band structures and d-band center of Ni-Fe-P,further increasing conductivity and optimizing intermediate adsorption energy.Our work not only proposes a valuable strategy to regulate the electron transfer and intermediate adsorption of electrocatalysts via RE atoms doping,but also provides a deep under-standing of regulation mechanism of metallic electrocatalysts for enhanced water splitting.
基金financially supported by the National Key Technology R&D Program of China(No.2021YFB3500801)
文摘Enhancing the activity of photocatalysts is a critical challenge for improving the photocatalytic degradation of contaminated wastewater.Here,a novel Ce single-atom-doped titanate nanotube photocatalyst(CeH_(2)Ti_(2)O_(5)·H_(2)O)was successfully synthesized using a onepot solvothermal method.Degradation experiments revealed that the optimal Ce doping ratio was 1.0%.The ultraviolet-visible diffuse reflectance spectroscopy results showed that the bandgap of the Ce-doped sample decreased from 3.02 to 2.87 eV,enhancing the absorption in the visible spectral range.At the same time,the BrunauerEmmett-Teller specific surface area increased from 63.68 to 88.95 m^(2)g^(-1).The 1.0%Ce-H_(2)Ti_(2)O_(5)·H_(2)O(HTC_(1))could degrade 99.04%of 100 mg L-1rhodamine B(RhB)after 40 min of visible-light irradiation.The degradation efficiency decreased by only 21.24%after five cycles.The results of free-radical quenching and electron spin resonance spectroscopy analyses indicated that HTC_(1)achieved efficient degradation of RhB through a direct hole oxidation mechanism.Compared with pure protonated titanate nanotubes(H_(2)Ti_(2)O_(5)·H_(2)O),HTC_(1)had a higher specific surface area,more electron traps,narrower bandgap,longer hole lifetime,and suppressed photogenerated charge recombination rate owing to the Ce single-atom doping.
