Transition metal phosphides(TMPs)have emerged as an alternative to precious metals as efficient and low-cost catalysts for water electrolysis.Elemental doping and morphology control are effective approaches to further...Transition metal phosphides(TMPs)have emerged as an alternative to precious metals as efficient and low-cost catalysts for water electrolysis.Elemental doping and morphology control are effective approaches to further improve the performance of TMPs.Herein,Fe-doped CoP nanoframes(Fe-CoP NFs)with specific open cage configuration were designed and synthesized.The unique nano-framework structured Fe-CoP material shows overpotentials of only 255 and 122 mV at 10 mA cm^(−2)for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER),respectively,overwhelming most transition metal phosphides.For overall water splitting,the cell voltage is 1.65 V for Fe-CoP NFs at a current density of 10 mA cm^(−2),much superior to what is observed for the classical nanocubic structures.Fe-CoP NFs show no activity degradation up to 100 h which contrasts sharply with the rapidly decaying performance of noble metal catalyst reference.The superior electrocatalytic performance of Fe-CoP NFs due to abundant accessible active sites,reduced kinetic energy barrier,and preferable*O-containing intermediate adsorption is demonstrated through experimental observations and theoretical calculations.Our findings could provide a potential method for the preparation of multifunctional material with hollow structures and offer more hopeful prospects for obtaining efficient earth-abundant catalysts for water splitting.展开更多
MoS_(2)is a promising electrocatalyst for hydrogen evolution reaction and a good candidate for cocatalyst to enhance the photoelectrochemical(PEC)performance of Si-based photoelectrode in aqueous electrolytes.The main...MoS_(2)is a promising electrocatalyst for hydrogen evolution reaction and a good candidate for cocatalyst to enhance the photoelectrochemical(PEC)performance of Si-based photoelectrode in aqueous electrolytes.The main challenge lies in the optimization of the microstructure of MoS_(2),to improve its catalytic activity and to construct a mechanically and chemically stable cocatalyst/Si photocathode.In this paper,a highly-ordered mesoporous MoS_(2)was synthesized and decorated onto a TiO_(2)protected p-silicon substrate.An additional TiO_(2)necking was introduced to strengthen the bonding between the MoS_(2)particles and the TiO_(2)layer.This meso-MoS_(2)/TiO_(2)/p-Si hybrid photocathode exhibited significantly enhanced PEC performance,where an onset potential of+0.06 V(versus RHE)and a current density of-1.8 mA/cm^(2)at 0 V(versus RHE)with a Faradaic efficiency close to 100%was achieved in 0.5 mol/L H_(2)SO_(4).Additionally,this meso-MoS_(2)/TiO_(2)/p-Si photocathode showed an excellent PEC ability and durability in alkaline media.This paper provides a promising strategy to enhance and protect the photocathode through high-performance surface cocatalysts.展开更多
基金the China Scholarship Council(CSC)for the financial support(202206230096)D.Yu would like to thank the CSC for the Doctor scholarship(202006360037)+1 种基金J.Dutta would like to acknowledge the partial financial support of VINNOVA project no.2021-02313.PZhang would like to acknowledge partial financial support from the National Natural Science Foundation of China(Nos 52111530187,51972210).
文摘Transition metal phosphides(TMPs)have emerged as an alternative to precious metals as efficient and low-cost catalysts for water electrolysis.Elemental doping and morphology control are effective approaches to further improve the performance of TMPs.Herein,Fe-doped CoP nanoframes(Fe-CoP NFs)with specific open cage configuration were designed and synthesized.The unique nano-framework structured Fe-CoP material shows overpotentials of only 255 and 122 mV at 10 mA cm^(−2)for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER),respectively,overwhelming most transition metal phosphides.For overall water splitting,the cell voltage is 1.65 V for Fe-CoP NFs at a current density of 10 mA cm^(−2),much superior to what is observed for the classical nanocubic structures.Fe-CoP NFs show no activity degradation up to 100 h which contrasts sharply with the rapidly decaying performance of noble metal catalyst reference.The superior electrocatalytic performance of Fe-CoP NFs due to abundant accessible active sites,reduced kinetic energy barrier,and preferable*O-containing intermediate adsorption is demonstrated through experimental observations and theoretical calculations.Our findings could provide a potential method for the preparation of multifunctional material with hollow structures and offer more hopeful prospects for obtaining efficient earth-abundant catalysts for water splitting.
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.51672174,51779139,51772190,and 51972210)the Advanced Energy Material and Technology Center of Shanghai Jiao Tong University,China.
文摘MoS_(2)is a promising electrocatalyst for hydrogen evolution reaction and a good candidate for cocatalyst to enhance the photoelectrochemical(PEC)performance of Si-based photoelectrode in aqueous electrolytes.The main challenge lies in the optimization of the microstructure of MoS_(2),to improve its catalytic activity and to construct a mechanically and chemically stable cocatalyst/Si photocathode.In this paper,a highly-ordered mesoporous MoS_(2)was synthesized and decorated onto a TiO_(2)protected p-silicon substrate.An additional TiO_(2)necking was introduced to strengthen the bonding between the MoS_(2)particles and the TiO_(2)layer.This meso-MoS_(2)/TiO_(2)/p-Si hybrid photocathode exhibited significantly enhanced PEC performance,where an onset potential of+0.06 V(versus RHE)and a current density of-1.8 mA/cm^(2)at 0 V(versus RHE)with a Faradaic efficiency close to 100%was achieved in 0.5 mol/L H_(2)SO_(4).Additionally,this meso-MoS_(2)/TiO_(2)/p-Si photocathode showed an excellent PEC ability and durability in alkaline media.This paper provides a promising strategy to enhance and protect the photocathode through high-performance surface cocatalysts.