Two-dimensional(2D)carbon nitride(CN)photocatalysts are attracting extensive attention owing to their excellent photocatalytic properties.In this study,we successfully prepared CN materials with heterogeneous structur...Two-dimensional(2D)carbon nitride(CN)photocatalysts are attracting extensive attention owing to their excellent photocatalytic properties.In this study,we successfully prepared CN materials with heterogeneous structures via hydrothermal treatment,high-temperature roasting,ball milling,sintering,and other processes.Benefitting from interface interactions in hybrid architectures,the CN photocatalysts exhibited high photocatalytic activity.The rate of hydrogen production using these CN photocatalysts reached 17028.82μmol h^(−1)g^(−1),and the apparent quantum efficiency was 11.2%at 420 nm.The ns-level time-resolved photoluminescence(PL)spectra provided information about the time-averaged lifetime of fluorescence charge carriers;the lifetime of the charge carriers causing the fluorescence of CN reached 9.99 ns.Significantly,the CN photocatalysts displayed satisfactory results in overall water splitting without the addition of sacrificial agents.The average hydrogen and oxygen production rates were 270.95μmol h^(−1)g^(−1)and 115.21μmol h^(−1)g^(−1)in 7 h,respectively,which were promising results for the applications of the catalysts in overall water splitting processes.We investigated the high efficiency of the prepared CN photocatalysts via a series of tests(UV-vis diffuse reflectance spectroscopy,photocurrent response measurements,PL emission spectroscopy,time-resolved PL spectroscopy,and Brunauer-Emmett-Teller analysis).Furthermore,the Mott-Schottky plot and current-voltage curve were acquired via electrochemical tests.The fabricated CN photocatalyst had a small p-n junction in its heterogeneous structure,which further enhanced its photocatalytic efficiency.Therefore,this work can promote the development of CN photocatalysts.展开更多
Photocatalytic overall water splitting is an interesting research topic in the field of energy and outer space exploration.Here,we designed a P/MoS_(2) composite photocatalyst with self-water-absorption performance by...Photocatalytic overall water splitting is an interesting research topic in the field of energy and outer space exploration.Here,we designed a P/MoS_(2) composite photocatalyst with self-water-absorption performance by compositing MoS_(2) nanosheets and polycrystalline black phosphorus nanosheets.The composite photocatalyst produced a sufficient amount of hydrogen in the absence of any precious metal.This also demonstrated photocatalytic overall water-splitting ability in the absence of any sacrificial agent.More interestingly,it effectively absorbed water and demonstrated good overall water-splitting performance under the simulated Mars conditions;the average hydrogen production rate was 17.68μmol h^(-1) g^(-1),and the oxygen production rate was 7.61μmol h^(-1) g^(-1) over a period of 70 h.A comprehensive investigation of the ability of the composite photocatalyst to absorb water and produce hydrogen was performed.展开更多
Hydrogen energy plays an important role in clean energy system and is considered the core energy source for future technological development owing to its lightweight nature,high calorific value,and clean combustion pr...Hydrogen energy plays an important role in clean energy system and is considered the core energy source for future technological development owing to its lightweight nature,high calorific value,and clean combustion products.The electrocatalytic conversion of water into hydrogen is considered a highly promising method.An electrocatalyst is indispensable in the electrocatalytic process,and finding an efficient electrocatalyst is essential.However,the current commercial electrocatalysts(such as Pt/C and Ru)are expensive;therefore,there is a need to find an inexpensive and efficient electrocatalyst with high stability,corrosion resistance,and high electrocatalytic efficiency.In this study,we developed a cost-effective bifunctional electrocatalyst by incorporating molybdenum into nickel sulfide(Ni_(3)S_(2))and subsequently tailoring its structure to achieve a one-dimensional(1D)needle-like configuration.The hydrogen production efficiency of nickel sulfide was improved by changing the ratio of Mo doping.By analyzing the electrochemical performance of different Mo-doped catalysts,we found that the Ni_(3)S_(2)-Mo-0.1 electrocatalyst exhibited the best electrocatalytic effect in 1 M KOH;at a current density of 10 mA cm^(-2),it exhibited overpotentials of 120 and 279 mV for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),respectively;at a higher current density of 100 mA cm^(-2),the HER and OER overpotentials were 396 and 495 mV,respectively.Furthermore,this electrocatalyst can be used in a two-electrode water-splitting system.Finally,we thoroughly investigated the mechanism of the overall water splitting of this electrocatalyst,providing valuable insights for future hydrogen production via overall-water-splitting.展开更多
Aqueous zinc-ion batteries are highly favored for their enhanced safety and reduced cost.However,there exist challenges including zinc dendrite,hydrogen evolution,and surface corrosion to be solved.Using electrolyte a...Aqueous zinc-ion batteries are highly favored for their enhanced safety and reduced cost.However,there exist challenges including zinc dendrite,hydrogen evolution,and surface corrosion to be solved.Using electrolyte additives is a highly convenient approach to solving zinc anode-related issues.Inspired by industrial corrosion protection,a trace amount of the corrosion inhibitor urotropine(URT)is used as an electrolyte additive to protect the zinc anode.Theoretical calculation and experimental analysis confirm the adsorption of URT molecules onto the surface of Zn,which inhibits hydrogen evolution.This adsorption further leads to the formation of an inorganic-organic bilayer solid electrolyte interface(SEI)on the surface of the zinc anode,effectively protecting the Zn anode from corrosion,hydrogen evolution and zinc dendrites.The presence of SEI enables symmetrical Zn//Zn cells to exhibit a long cycling performance of 1750 h at 1mA/cm^(2)and an average coulombic efficiency of 99.0%at 1mA/cm^(2)in Zn//Cu cells.After being coupled with polyaniline(PANI),the Zn//PANI full battery displays excellent cycle stability and specific capacity.展开更多
g-C_(3)N_(4) have been widely used in the fields of photocatalytic hydrogen production,photocatalytic degradation of dyes and oxidative degradation of toxic gases due to their excellent performance.It has attracted ex...g-C_(3)N_(4) have been widely used in the fields of photocatalytic hydrogen production,photocatalytic degradation of dyes and oxidative degradation of toxic gases due to their excellent performance.It has attracted extensive attention in recent years due to its highly efficient photocatalytic capacity of hydrogen generation,water oxidation,carbon dioxide reduction and degradation of organic pollutants.Because of the abundant carbon and nitrogen composition of the earth,large-scale production and industrial applications of this material are possible.The modification of this material makes its performance more excellent so that this new material can obtain a steady stream of vitality.These outstanding works have become important materials and milestones on the road to mankind's photocatalytic hydrogen production.This review will begin with the basic idea of designing,synthesizing and improving g-C_(3)N_(4) based photocatalytic materials,and introduce the latest development of g-C_(3)N_(4) photocatalysts in hydrogen production from four aspects of controlling the carbon/nitrogen ratio,morphology,element doping and heterojunction structure of g-C_(3)N_(4) materials.展开更多
Carbon nitride(CN) photocatalysts have attracted much attention due to their excellent photocatalytic properties.And hydrothermal fluorination is a common method to improve the photocatalytic effect of CN photocatalys...Carbon nitride(CN) photocatalysts have attracted much attention due to their excellent photocatalytic properties.And hydrothermal fluorination is a common method to improve the photocatalytic effect of CN photocatalyst.Here,the influence of the band gap was first revealed of fluorination and hydroxylation of CN photocatalyst based on the first theoretical principle.Here,the effect of fluorination and hydroxylation on the CN band gap was discussed for the first time using the first theoretical principle.With F atoms and OH doping,the band gap of CN was significantly improved,conduction band and valence band moved up.Then,F-CN photocatalyst with F atoms and OH was successfully synthesized by a hydrothermal fluorinated method.Next,the reasons why F-CN photocatalyst was more effective than that of traditional CN photocatalyst were fully discussed.From the photocatalytic effect of photocatalyst(12,593.2 μmolg^(-1) h^(-1)to the morphology(super-small nanosheets),structure(homojunctions),composition(metal-free),specific surface area(54.1 m^(2)/g),visible light absorption response(AQE is10.9% at 420 nm) and photo-induced carrier life(14.13 ns).Therefore,this work has a great guiding effect on the development of CN photocatalyst.展开更多
Flexible aqueous energy storage devices with high security and flexibility are crucial for the progress of wearable energy storage.Particularly,aqueous rechargeable Ni-Fe batteries owning a large theoretical capacity,...Flexible aqueous energy storage devices with high security and flexibility are crucial for the progress of wearable energy storage.Particularly,aqueous rechargeable Ni-Fe batteries owning a large theoretical capacity,low cost and outstanding safety characteristics have emerged as a promising candidate for flexible aqueous energy storage devices.Herein,Cu-doped Fe_(3)O_(4)(CFO)with 3D coral structure was prepared by doping Cu^(2+) based on Fe_(3)O_(4)nanosheets(FO).Furthermore,the Fe-based anode material(CFPO)grown on carbon fibers was obtained by reconstructing the surface of CFO to form a low-crystallization shell which can enhance the ion transport.Excitingly,the newly developed CFPO electrode as an innovative anode material further exhibited a high capacity of 117.5 mAh g^(-1)(or 423 F g^(-1))at 1 A g^(-1).Then,the assembled aqueous Ni-Fe batteries with a high cell-voltage output of 1.6 V deliver a high capacity of 49.02 mAh g^(-1) at 1 A g^(-1) and retention ratio of 96.8%for capacitance after 10000 continuous cycles.What’s more,the aqueous quasi-solid-state batteries present a remarkable maximal energy density of 45.6 Wh kg^(-1) and a power density of 12 kW kg^(-1).This work provides an innovative and feasible way and optimization idea for the design of high-performance Fe-based anodes,and may promote the development of a new generation of flexible aqueous Ni-Fe batteries.展开更多
Zinc-ion batteries are under current research focus because of their uniqueness in low cost and high safety.However,the pursuing of high-performance cathode materials of aqueous Zinc ion batteries(AZBs)with low cost,h...Zinc-ion batteries are under current research focus because of their uniqueness in low cost and high safety.However,the pursuing of high-performance cathode materials of aqueous Zinc ion batteries(AZBs)with low cost,high energy density and long cycle life has become the key problem to be solved.Herein we synthesized a series of amorphous nickel borate(AM-NiBO)nanosheets by varying corrosion time with in-situ electrochemical corrosion method.The AM-NiBO-T13 as electrode material possesses a high areal capacity of 0.65 m Ah/cm^(2) with the capacity retention of 95.1%after 2000 cycles.In addition,the assembled AM-NiBO-T13//Zn provides high energy density(0.77 m Wh/cm^(2) at 1.76 m W/cm^(2)).The high areal capacity and better cycling performance can be owing to the amorphous nanosheets structure and the stable coordination characteristics of boron and oxygen in borate materials.It shows that amorphous nickel borate nanosheets have great prospects in the field of energy storage.展开更多
Developing efficient electrocatalysts for hydrogen evolution reaction(HER) is of great importance in contemporary water electrolysis technology. Here, a novel hierarchically sea urchin-like electrocatalyst(Mo_(4)O_(11...Developing efficient electrocatalysts for hydrogen evolution reaction(HER) is of great importance in contemporary water electrolysis technology. Here, a novel hierarchically sea urchin-like electrocatalyst(Mo_(4)O_(11)-MoS_(2)-VO_(2)) is synthesized by hydrothermal deposition and post-annealing strategy. The optimized electrocatalyst behaves as a high active hydrogen evolution electrode in 0.5 mol/L H_(2)SO_(4). This electrode needs overpotential of only 43 m V to achieve 10 m A/cm^(2)with a Tafel slope of 37 m V/dec and maintains its catalytic activity for at least 36 h. Better than most previously reported non-noble metal electrocatalysts anchored on carbon cloth. It is worth mentioning that the hierarchical sea urchin-like structure promotes the redistribution of electrons and provides more catalytic active sites. This strategy shows a way for the construction of inexpensive non-noble metal electrocatalysts in the future.展开更多
文摘Two-dimensional(2D)carbon nitride(CN)photocatalysts are attracting extensive attention owing to their excellent photocatalytic properties.In this study,we successfully prepared CN materials with heterogeneous structures via hydrothermal treatment,high-temperature roasting,ball milling,sintering,and other processes.Benefitting from interface interactions in hybrid architectures,the CN photocatalysts exhibited high photocatalytic activity.The rate of hydrogen production using these CN photocatalysts reached 17028.82μmol h^(−1)g^(−1),and the apparent quantum efficiency was 11.2%at 420 nm.The ns-level time-resolved photoluminescence(PL)spectra provided information about the time-averaged lifetime of fluorescence charge carriers;the lifetime of the charge carriers causing the fluorescence of CN reached 9.99 ns.Significantly,the CN photocatalysts displayed satisfactory results in overall water splitting without the addition of sacrificial agents.The average hydrogen and oxygen production rates were 270.95μmol h^(−1)g^(−1)and 115.21μmol h^(−1)g^(−1)in 7 h,respectively,which were promising results for the applications of the catalysts in overall water splitting processes.We investigated the high efficiency of the prepared CN photocatalysts via a series of tests(UV-vis diffuse reflectance spectroscopy,photocurrent response measurements,PL emission spectroscopy,time-resolved PL spectroscopy,and Brunauer-Emmett-Teller analysis).Furthermore,the Mott-Schottky plot and current-voltage curve were acquired via electrochemical tests.The fabricated CN photocatalyst had a small p-n junction in its heterogeneous structure,which further enhanced its photocatalytic efficiency.Therefore,this work can promote the development of CN photocatalysts.
基金supported by the National Natural Science Foundation of China(Grant No.51802177)Independent Cultivation Program of the Innovation Team of Jinan City(Grant No.2019GXRC011)Natural Science Foundation of Shandong Province(Grant No.ZR2018BEM019).
文摘Photocatalytic overall water splitting is an interesting research topic in the field of energy and outer space exploration.Here,we designed a P/MoS_(2) composite photocatalyst with self-water-absorption performance by compositing MoS_(2) nanosheets and polycrystalline black phosphorus nanosheets.The composite photocatalyst produced a sufficient amount of hydrogen in the absence of any precious metal.This also demonstrated photocatalytic overall water-splitting ability in the absence of any sacrificial agent.More interestingly,it effectively absorbed water and demonstrated good overall water-splitting performance under the simulated Mars conditions;the average hydrogen production rate was 17.68μmol h^(-1) g^(-1),and the oxygen production rate was 7.61μmol h^(-1) g^(-1) over a period of 70 h.A comprehensive investigation of the ability of the composite photocatalyst to absorb water and produce hydrogen was performed.
基金supported by the National Natural Science Foundation of China(No.51802177)the Joint Funds of the National Natural Science Foundation of China(No.U22A20140)State Key Laboratory of Powder Metallurgy,Central South University,Changsha,China.
文摘Hydrogen energy plays an important role in clean energy system and is considered the core energy source for future technological development owing to its lightweight nature,high calorific value,and clean combustion products.The electrocatalytic conversion of water into hydrogen is considered a highly promising method.An electrocatalyst is indispensable in the electrocatalytic process,and finding an efficient electrocatalyst is essential.However,the current commercial electrocatalysts(such as Pt/C and Ru)are expensive;therefore,there is a need to find an inexpensive and efficient electrocatalyst with high stability,corrosion resistance,and high electrocatalytic efficiency.In this study,we developed a cost-effective bifunctional electrocatalyst by incorporating molybdenum into nickel sulfide(Ni_(3)S_(2))and subsequently tailoring its structure to achieve a one-dimensional(1D)needle-like configuration.The hydrogen production efficiency of nickel sulfide was improved by changing the ratio of Mo doping.By analyzing the electrochemical performance of different Mo-doped catalysts,we found that the Ni_(3)S_(2)-Mo-0.1 electrocatalyst exhibited the best electrocatalytic effect in 1 M KOH;at a current density of 10 mA cm^(-2),it exhibited overpotentials of 120 and 279 mV for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),respectively;at a higher current density of 100 mA cm^(-2),the HER and OER overpotentials were 396 and 495 mV,respectively.Furthermore,this electrocatalyst can be used in a two-electrode water-splitting system.Finally,we thoroughly investigated the mechanism of the overall water splitting of this electrocatalyst,providing valuable insights for future hydrogen production via overall-water-splitting.
基金financially supported by Joint Funds of the National Natural Science Foundation of China(No.U22A20140)the National Natural Science Foundation of China(No.22379062)+1 种基金supported by Shenzhen Stable Support Plan Program for Higher Education Institutions Research Program(No.20220816131408001)Shenzhen Science and Technology Program(No.JCYJ20230807091802006)。
文摘Aqueous zinc-ion batteries are highly favored for their enhanced safety and reduced cost.However,there exist challenges including zinc dendrite,hydrogen evolution,and surface corrosion to be solved.Using electrolyte additives is a highly convenient approach to solving zinc anode-related issues.Inspired by industrial corrosion protection,a trace amount of the corrosion inhibitor urotropine(URT)is used as an electrolyte additive to protect the zinc anode.Theoretical calculation and experimental analysis confirm the adsorption of URT molecules onto the surface of Zn,which inhibits hydrogen evolution.This adsorption further leads to the formation of an inorganic-organic bilayer solid electrolyte interface(SEI)on the surface of the zinc anode,effectively protecting the Zn anode from corrosion,hydrogen evolution and zinc dendrites.The presence of SEI enables symmetrical Zn//Zn cells to exhibit a long cycling performance of 1750 h at 1mA/cm^(2)and an average coulombic efficiency of 99.0%at 1mA/cm^(2)in Zn//Cu cells.After being coupled with polyaniline(PANI),the Zn//PANI full battery displays excellent cycle stability and specific capacity.
基金supported by the National Natural Science Foundation of China(Nos.51672109,51802177)the Independent Cultivation Program of Innovation Team of Ji’nan City(No.2019GXRC011)Natural Science Foundation of Shandong Province(No.ZR2018BEM019)。
文摘g-C_(3)N_(4) have been widely used in the fields of photocatalytic hydrogen production,photocatalytic degradation of dyes and oxidative degradation of toxic gases due to their excellent performance.It has attracted extensive attention in recent years due to its highly efficient photocatalytic capacity of hydrogen generation,water oxidation,carbon dioxide reduction and degradation of organic pollutants.Because of the abundant carbon and nitrogen composition of the earth,large-scale production and industrial applications of this material are possible.The modification of this material makes its performance more excellent so that this new material can obtain a steady stream of vitality.These outstanding works have become important materials and milestones on the road to mankind's photocatalytic hydrogen production.This review will begin with the basic idea of designing,synthesizing and improving g-C_(3)N_(4) based photocatalytic materials,and introduce the latest development of g-C_(3)N_(4) photocatalysts in hydrogen production from four aspects of controlling the carbon/nitrogen ratio,morphology,element doping and heterojunction structure of g-C_(3)N_(4) materials.
基金supported by the National Natural Science Foundation of China(Nos.51802177,51672109)Independent Cultivation Program of Innovation Team of Ji’nan City(No.2019GXRC011)+1 种基金the Major Basic Program of the Natural Science Foundation of Shandong Province(Contract ZR2018ZC0842)Natural Science Foundation of Shandong Province(No.ZR2018BEM019)。
文摘Carbon nitride(CN) photocatalysts have attracted much attention due to their excellent photocatalytic properties.And hydrothermal fluorination is a common method to improve the photocatalytic effect of CN photocatalyst.Here,the influence of the band gap was first revealed of fluorination and hydroxylation of CN photocatalyst based on the first theoretical principle.Here,the effect of fluorination and hydroxylation on the CN band gap was discussed for the first time using the first theoretical principle.With F atoms and OH doping,the band gap of CN was significantly improved,conduction band and valence band moved up.Then,F-CN photocatalyst with F atoms and OH was successfully synthesized by a hydrothermal fluorinated method.Next,the reasons why F-CN photocatalyst was more effective than that of traditional CN photocatalyst were fully discussed.From the photocatalytic effect of photocatalyst(12,593.2 μmolg^(-1) h^(-1)to the morphology(super-small nanosheets),structure(homojunctions),composition(metal-free),specific surface area(54.1 m^(2)/g),visible light absorption response(AQE is10.9% at 420 nm) and photo-induced carrier life(14.13 ns).Therefore,this work has a great guiding effect on the development of CN photocatalyst.
基金supported by the National Natural Science Foundation of China(Grant Nos.51802177)Independent Cultivation Program of Innovation Team of Ji’nan City(Grant No.2019GXRC011)。
文摘Flexible aqueous energy storage devices with high security and flexibility are crucial for the progress of wearable energy storage.Particularly,aqueous rechargeable Ni-Fe batteries owning a large theoretical capacity,low cost and outstanding safety characteristics have emerged as a promising candidate for flexible aqueous energy storage devices.Herein,Cu-doped Fe_(3)O_(4)(CFO)with 3D coral structure was prepared by doping Cu^(2+) based on Fe_(3)O_(4)nanosheets(FO).Furthermore,the Fe-based anode material(CFPO)grown on carbon fibers was obtained by reconstructing the surface of CFO to form a low-crystallization shell which can enhance the ion transport.Excitingly,the newly developed CFPO electrode as an innovative anode material further exhibited a high capacity of 117.5 mAh g^(-1)(or 423 F g^(-1))at 1 A g^(-1).Then,the assembled aqueous Ni-Fe batteries with a high cell-voltage output of 1.6 V deliver a high capacity of 49.02 mAh g^(-1) at 1 A g^(-1) and retention ratio of 96.8%for capacitance after 10000 continuous cycles.What’s more,the aqueous quasi-solid-state batteries present a remarkable maximal energy density of 45.6 Wh kg^(-1) and a power density of 12 kW kg^(-1).This work provides an innovative and feasible way and optimization idea for the design of high-performance Fe-based anodes,and may promote the development of a new generation of flexible aqueous Ni-Fe batteries.
基金supported by the Independent Cultivation Program of Innovation Team of Ji’nan City(No.2019GXRC011)。
文摘Zinc-ion batteries are under current research focus because of their uniqueness in low cost and high safety.However,the pursuing of high-performance cathode materials of aqueous Zinc ion batteries(AZBs)with low cost,high energy density and long cycle life has become the key problem to be solved.Herein we synthesized a series of amorphous nickel borate(AM-NiBO)nanosheets by varying corrosion time with in-situ electrochemical corrosion method.The AM-NiBO-T13 as electrode material possesses a high areal capacity of 0.65 m Ah/cm^(2) with the capacity retention of 95.1%after 2000 cycles.In addition,the assembled AM-NiBO-T13//Zn provides high energy density(0.77 m Wh/cm^(2) at 1.76 m W/cm^(2)).The high areal capacity and better cycling performance can be owing to the amorphous nanosheets structure and the stable coordination characteristics of boron and oxygen in borate materials.It shows that amorphous nickel borate nanosheets have great prospects in the field of energy storage.
基金supported by the National Natural Science Foundation of China (No. 51802177)Independent Cultivation Program of Innovation Team of Ji nan City (No. 2019GXRC011)Introduction and Cultivation Plan of Young Innovative Talents in Colleges and Universities of Shandong Province,Shandong Provincial Natural Science Foundation (No. ZR^(2)020ME052)。
文摘Developing efficient electrocatalysts for hydrogen evolution reaction(HER) is of great importance in contemporary water electrolysis technology. Here, a novel hierarchically sea urchin-like electrocatalyst(Mo_(4)O_(11)-MoS_(2)-VO_(2)) is synthesized by hydrothermal deposition and post-annealing strategy. The optimized electrocatalyst behaves as a high active hydrogen evolution electrode in 0.5 mol/L H_(2)SO_(4). This electrode needs overpotential of only 43 m V to achieve 10 m A/cm^(2)with a Tafel slope of 37 m V/dec and maintains its catalytic activity for at least 36 h. Better than most previously reported non-noble metal electrocatalysts anchored on carbon cloth. It is worth mentioning that the hierarchical sea urchin-like structure promotes the redistribution of electrons and provides more catalytic active sites. This strategy shows a way for the construction of inexpensive non-noble metal electrocatalysts in the future.
