Developing efficient and durable oxygen evolution reaction(OER)catalysts under acidic conditions is crucial for green hydrogen production.Constructing heterogeneous interface structures represents the most promising s...Developing efficient and durable oxygen evolution reaction(OER)catalysts under acidic conditions is crucial for green hydrogen production.Constructing heterogeneous interface structures represents the most promising strategy to overcome the intrinsic activity limitations of electrocatalysts.Here,a catalyst with crystalline-amorphous heterostructure(RuO_(2)/Cr_(2)O_(3))exhibiting enhanced performance in the acidic OER has been prepared,which achieves a low overpotential of 218 mV at 10 mA cm^(-2).X-ray photoelectron spectroscopy(XPS)and X-ray absorption spectroscopy(XAS)analyses indicate that the electron density of Ru is modulated by the interaction with Cr,leading to improved Ru-O bonding characteristics.The heterostructure effectively reduces the charge transfer resistance at the interface between the crystalline and amorphous phases and facilitates the adsorption/desorption of OER intermediates.In situ Raman spectroscopy further reveals that the Ru-O bond interactions are significantly enhanced due to the formation of a heterogeneous interface,which stabilizes the dissolution of Ru species at elevated potential.Mass spectrometry analysis confirmed that lattice oxygen participation was inhibited,contributing to improvements in the durability of the OER,resulting in catalyst stability of over 30 hours at 10 mA cm^(-2).This study presents a feasible strategy for the design and development of catalysts with enhanced activity and stability.展开更多
Semiconductor photocatalysis provides a promising potential solution to the challenging issue of clean energy production.Construction of multijunction systems is an effective strategy to overcome the serious drawbacks...Semiconductor photocatalysis provides a promising potential solution to the challenging issue of clean energy production.Construction of multijunction systems is an effective strategy to overcome the serious drawbacks of fast charge recombination and the limited visible-light absorption of semiconductor photocatalysts.Here,we report a novel quaternary heterogeneous photocatalyst fabricated by loading Ag nanoparticles onto ZnO nanowires and subsequent simultaneous formation of core/shell structured ZnO@ZnS and Ag@Ag_(2)S heterojunctions via a one-step anion-exchange sulfuration reaction process.The resulting four-component ZnO@ZnS/Ag@Ag_(2)S multijunction photocatalyst exhibits a high hydrogen evolution activity(140.3μmol g^(-1))under simulated solar light irradiation in 5 h,far exceeding those of bare ZnO(30.8μmol g^(-1)),ZnO@ZnS(92.8μmol g^(-1))and ZnO/Ag(45.1μmol g^(-1))counterparts.The enhanced photocatalytic activity can be attributed to the synergetic effect of the formation of both Z-scheme and type II core/shell heterojunctions,favoring light absorption and separation of photogenerated electron-hole pairs in the composite.This work provides a facile,controlled method for the fabrication of multicomponent heterostructures used for efficient solar water splitting.展开更多
基金supported by the State Key Laboratory of Powder Metallurgy,the Open Project of Yunnan Precious Metals Laboratory Co.,Ltd(YPML-2023050264 and YPML-2023050204)the National Natural Science Foundation of China(12074435)+2 种基金the Science and Technology Planning Project of Yunnan Province(202302AH_(3)60001)the China Postdoctoral Science Foundation(2024M763694 and 2023M743941)the Postdoctoral Fellowship Program(Grade B)of the China Postdoctoral Science Foundation(GZB20240859 and GZB20240858).
文摘Developing efficient and durable oxygen evolution reaction(OER)catalysts under acidic conditions is crucial for green hydrogen production.Constructing heterogeneous interface structures represents the most promising strategy to overcome the intrinsic activity limitations of electrocatalysts.Here,a catalyst with crystalline-amorphous heterostructure(RuO_(2)/Cr_(2)O_(3))exhibiting enhanced performance in the acidic OER has been prepared,which achieves a low overpotential of 218 mV at 10 mA cm^(-2).X-ray photoelectron spectroscopy(XPS)and X-ray absorption spectroscopy(XAS)analyses indicate that the electron density of Ru is modulated by the interaction with Cr,leading to improved Ru-O bonding characteristics.The heterostructure effectively reduces the charge transfer resistance at the interface between the crystalline and amorphous phases and facilitates the adsorption/desorption of OER intermediates.In situ Raman spectroscopy further reveals that the Ru-O bond interactions are significantly enhanced due to the formation of a heterogeneous interface,which stabilizes the dissolution of Ru species at elevated potential.Mass spectrometry analysis confirmed that lattice oxygen participation was inhibited,contributing to improvements in the durability of the OER,resulting in catalyst stability of over 30 hours at 10 mA cm^(-2).This study presents a feasible strategy for the design and development of catalysts with enhanced activity and stability.
基金Shenzhen Science and Technology Innovation Committee(Grant No.JCYJ20170817111443306,JCYJ20170412154335393 and KQTD2016022619584022)Southern University of Science and Technology(Grant No.G01296001)+1 种基金Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control(Grant No.2017B030301012)NSFC(No.51802143)。
文摘Semiconductor photocatalysis provides a promising potential solution to the challenging issue of clean energy production.Construction of multijunction systems is an effective strategy to overcome the serious drawbacks of fast charge recombination and the limited visible-light absorption of semiconductor photocatalysts.Here,we report a novel quaternary heterogeneous photocatalyst fabricated by loading Ag nanoparticles onto ZnO nanowires and subsequent simultaneous formation of core/shell structured ZnO@ZnS and Ag@Ag_(2)S heterojunctions via a one-step anion-exchange sulfuration reaction process.The resulting four-component ZnO@ZnS/Ag@Ag_(2)S multijunction photocatalyst exhibits a high hydrogen evolution activity(140.3μmol g^(-1))under simulated solar light irradiation in 5 h,far exceeding those of bare ZnO(30.8μmol g^(-1)),ZnO@ZnS(92.8μmol g^(-1))and ZnO/Ag(45.1μmol g^(-1))counterparts.The enhanced photocatalytic activity can be attributed to the synergetic effect of the formation of both Z-scheme and type II core/shell heterojunctions,favoring light absorption and separation of photogenerated electron-hole pairs in the composite.This work provides a facile,controlled method for the fabrication of multicomponent heterostructures used for efficient solar water splitting.
