The sulfur phase in high sulfur-containing bauxite was studied by an X-ray diffraction analysis and a chemistry quantitative analysis.The methods for the removal of different shaped sulfur were also discussed.The resu...The sulfur phase in high sulfur-containing bauxite was studied by an X-ray diffraction analysis and a chemistry quantitative analysis.The methods for the removal of different shaped sulfur were also discussed.The results show that sulfur phases in high sulfur-containing bauxites exist in the main form of sulfide sulfur (pyrite) or sulfate sulfur,and the main sulfur forms of bauxites from different regions are not the same.Through a combination of an X-ray diffraction analysis and a chemistry quantitative analysis,the sulfur phases of high sulfur-containing bauxite could be accurately investigated.Deciding the main sulfur form of high sulfur-containing bauxite could provide theoretical instruction for choosing methods for the removal of sulfur from bauxite,and an oxidizing-roasting process is an effective way to remove sulfide sulfur from high sulfur-containing bauxite,the content of S^2-in crude ore in the digestion liquor is above 1.7 g/L,but in the roasted ore digestion liquor,it is below 0.18 g/L.Using the sodium carbonate solution washing technology to wash bauxite can effectively remove sulfate sulfur,the content of the total sulfur in ore is lowered to below 0.2% and can meet the production requirements for the sulfur content.展开更多
As one of the most appealing and attractive technologies, photocatalysis is widely used as a promising method to circumvent the environmental and energy problems. Due to its chemical stability and unique physicochemic...As one of the most appealing and attractive technologies, photocatalysis is widely used as a promising method to circumvent the environmental and energy problems. Due to its chemical stability and unique physicochemical, graphitic carbon nitride (g-C3N4) has become research hotspots in the community. However, g-C3N4 photocatalyst still suffers from many problems, resulting in unsatisfactory photocatalytic activity such as low specific surface area, high charge recombination and insufficient visible light utilization. Since 2009, g-C3N4-based heterostructures have attracted the attention of scientists worldwide for their greatly enhanced photocatalytic performance. Overall, this review summarizes the recent advances of g-C3N4-based nanocomposites modified with transition metal sulfide (TMS), including (1) preparation of pristine g-C3N4,(2) modification strategies of g-C3N4,(3) design principles of TMS-modified g-C3N4 heterostructured photocatalysts, and (4) applications in energy conversion. What is more, the characteristics and transfer mechanisms of each classification of the metal sulfide heterojunction system will be critically reviewed, spanning from the following categories:(1) Type I heterojunction,(2) Type II heterojunction,(3) p-n heterojunction,(4) Schottky junction and (5) Z-scheme heterojunction. Apart from that, the application of g-C3N4-based heterostructured photocatalysts in H2 evolution, CO2 reduction, N2 fixation and pollutant degradation will also be systematically presented. Last but not least, this review will conclude with invigorating perspectives, limitations and prospects for further advancing g-C3N4-based heterostructured photocatalysts toward practical benefits for a sustainable future.展开更多
Expanding the optical absorption range of photocatalysts is still a key endeavor in graphitic carbon nitride(g-C_(3)N_(4))studies.Here,we report on a novel thiophene group extending the optical property,which is assig...Expanding the optical absorption range of photocatalysts is still a key endeavor in graphitic carbon nitride(g-C_(3)N_(4))studies.Here,we report on a novel thiophene group extending the optical property,which is assigned to n-π^(*)electronic transitions involving the two lone pairs on sulfur(TLPS).The as-prepared samples,denoted as CN-ThAx(where x indicates the amount of ThA added,mg),showed an additional absorption above 500 nm as compared to pristine g-C_(3)N_(4).Further,the thiophene group enhanced charge carrier separation to suppress e‒/h+pair recombination.The experimental results suggest that the thiophene group can obstruct the polymerization of melem to generate a large plane,thus exposing the lone electron pairs on the sulfur.The photocatalytic activity was evaluated in the decomposition of bisphenol A and H2 evolution.Compared with g-C_(3)N_(4),the optimized CN-ThA_(30) sample led to a 6.6-and 2-fold enhancement of the degradation and H2 generation rates,respectively.The CN-ThA_(30) sample allowed for synchronous H2 production and BPA decomposition.展开更多
Two-dimensional materials(2D)with unique physicochemical properties have been widely studied for their use in many applications,including as hydrogen evolution catalysts to improve the efficiency of water splitting.Re...Two-dimensional materials(2D)with unique physicochemical properties have been widely studied for their use in many applications,including as hydrogen evolution catalysts to improve the efficiency of water splitting.Recently,typical 2D materials MoS2,graphene,MXenes,and black phosphorus have been widely investigated for their application in the hydrogen evolution reaction(HER).In this review,we summarize three efficient strategies—defect engineering,heterostructure formation,and heteroatom doping—for improving the HER performance of 2D catalysts.The d-band theory,density of states,and Fermi energy level are discussed to provide guidance for the design and construction of novel 2D materials.The challenges and prospects of 2D materials in the HER are also considered.展开更多
Activated carbon/nanosized CdS/chitosan(AC/n-CdS/CS) composites as adsorbent and photoactive catalyst were prepared under low temperature(≤60 ℃) and ambient pressure.Methyl orange(MO) was chosen as a model pollutant...Activated carbon/nanosized CdS/chitosan(AC/n-CdS/CS) composites as adsorbent and photoactive catalyst were prepared under low temperature(≤60 ℃) and ambient pressure.Methyl orange(MO) was chosen as a model pollutant to evaluate synergistic effect of adsorption and photocatalytic decolorization by this innovative photocatalyst under visible light irradiation.Effects of various parameters such as catalyst amount,initial MO concentration,solution pH and reuse of catalyst on the decolorization of MO were investigated to optimize operational conditions.The decolorization of MO catalyzed by AC/n-CdS/CS fits the Langmuir-Hinshelwood kinetics model,and a surface reaction,where the dyes are absorbed,is the controlling step of the process.Decolorization efficiency of MO is improved with the increase in catalyst amount within a certain range.The photodecolorization of MO is more efficient in acidic media than alkaline media.The decolorization efficiency of MO is still higher than 84% after five cycles and 60 min under visible light irradiation,which confirms the reusability of AC/n-CdS/CS composite catalyst.展开更多
The denitrifying sulfide removal(DSR) process with bio-granules comprising both heterotrophic and autotrophic denitrifiers can simultaneously convert nitrate, sulfide and acetate species into di-nitrogen gas, elementa...The denitrifying sulfide removal(DSR) process with bio-granules comprising both heterotrophic and autotrophic denitrifiers can simultaneously convert nitrate, sulfide and acetate species into di-nitrogen gas, elemental sulfur and carbon dioxide, respectively, at high loading rates. This study has determined that the reaction rate of sulfide oxidized into sulfur could be enhanced in the presence of 1,2-naphthoquinone-4-sulphonate(NQS). The presence of NQS mitigated the inhibition effects of sulfide species on denitrification. Furthermore, the reaction rates of nitrate and acetate to nitrogen gas and CO_2, respectively, were also promoted in the presence of NQS, thereby enhancing the performance of DSR granules. The advantages and disadvantages of applying the NQS-DSR process are discussed.展开更多
There are sulfate and chloride ions corrosion and carbonation to concrete in coal mine. Based on taking test of accelerated carbonation, corrosion of 3.5% weight of NaCl solution and 5% weight of Na2SO4 solution of co...There are sulfate and chloride ions corrosion and carbonation to concrete in coal mine. Based on taking test of accelerated carbonation, corrosion of 3.5% weight of NaCl solution and 5% weight of Na2SO4 solution of coal mine concretes, durability of con- cretes which include spray concrete of C20,high performance concretes of C30 and C50 and effect of fly ash on durability have been studied. Results suggest that the coal mineral high performance concretes show good resistance capacities of carbonation, sulfate and chloride corrosion to meet the coal mine construction. And the higher the strength grade is, the better the resistance capacity of corrosion of carbonation is, chloride and sulfate. Moreover, fly ash improves resistance capacity of high performance concrete(HPC) to chloride and sulfate but decreases the resistance capacity of C30’s to carbonation and average dynamic modulus.展开更多
Reversible oxygen reaction plays a crucial role in rechargeable battery systems,but it is limited by the slow reaction kinetics.Herein,the ionic modulation of cobalt pentlandite coupled with nitrogen‐doped bowl‐like...Reversible oxygen reaction plays a crucial role in rechargeable battery systems,but it is limited by the slow reaction kinetics.Herein,the ionic modulation of cobalt pentlandite coupled with nitrogen‐doped bowl‐like hollow carbon sphere is well designed on octahedral and tetrahedral sites.The robust FexCo9−xS8‐NHCS‐V with iron replacing at the octahedron possesses prolonged metal sulfur bond and exhibits excellent bifunctional electrocatalytic performance towards oxygen reduction reaction(ORR,E_(1/2)=0.80 V vs.RHE)and excellent oxygen evolution reaction(OER,E_(j=10)=1.53 V vs.RHE)in 0.1 mol/L KOH.Accordingly,a rechargeable Zn‐air battery of Fe_(x)Co_(9−x)S_(8)‐NHCS‐V cathode endows high energy efficiency(102 mW cm^(−2)),and a microbial fuel cell achieves a high‐power density(791±42 mW m^(−2)),outperforming the benchmark Pt/C catalyst.展开更多
The catalytic oxidization of CS2 over atmospheric particles and some oxide catalysts was explored through FT-IR, MS and a fixed-bed stainless steel reactor. The results show that atmospheric particles and some oxide c...The catalytic oxidization of CS2 over atmospheric particles and some oxide catalysts was explored through FT-IR, MS and a fixed-bed stainless steel reactor. The results show that atmospheric particles and some oxide catalysts exhibited considerable oxidizing activities for CS2 at ambient temperature. The reaction products are mainly COS and elemental sulfur, even CO2 on some catalysts. Among the catalysts, CaO has the strongest catalytic activity for oxidizing CS2. Fe2O3 is weaker than CaO. The catalytic activity for Al2O3 reduces considerably compared with the former two catalysts, and SiO2 the weakest. Atmospheric particle samples’ catalytic activity is between Fe2O3’s and Al2O3’s. The atmospheric particle sample collected mainly consists of Ca(Al2Si2O8) · 4H2O, which is also the main component of cement. COS, the main product, is formed by the catalytic oxidization of CS2 with adsorbed “molecular” oxygen over the catalysts’ surfaces. The concentration of adsorbed oxygen over catalysts’ surfaces may be the key factor contributed to the oxidizing activity. It is indicated that CS2 could be catalytically oxidized over atmospheric particles, which induced that this reaction may be another important source of atmospheric COS from CS2.展开更多
Hydrogen, serving as a clean, sustainable energy source, may be mainly produced from electrolysis water. Herein, we report cobalt disulphide encapsulated in self-catalyzed carbon nanotubes (S, N-CNTs/ CoS2@Co) servi...Hydrogen, serving as a clean, sustainable energy source, may be mainly produced from electrolysis water. Herein, we report cobalt disulphide encapsulated in self-catalyzed carbon nanotubes (S, N-CNTs/ CoS2@Co) serving as a bifunctional catalyst, which exhibits excellent hydrogen evolution reaction perfor-mance (10.0 mAcm^-2 at 0.112 V, and low Tafel slope for 104.9 mV dec^-1 ) and oxygen evolution reaction performance (10.0 mAcm^-2 at 1.57 V, and low Tafel slope for 76.1 mV dec^-1), meanwbile with a strong stability at various current densities. In-depth study reveals that the excellent catalytic properties can be mainly attributed to the increased catalytic sites induced by S, N co-doping, the improved electronic con-ductivity derived from the carbon nanotubes, and Mott-Schottky effect between the metal cobalt and semiconductive cobalt disulfide. Notably, when the bifunctional catalysts are applied to overall water splitting, a low potential of 1.633 V at the current density of 10.0 mAcm^-2 is achieved, which can com-pete with the precious metal catalyst benchmarks in alkaline media, demonstrating its promising prac-ticability in the realistic water splitting application. This work elucidates a practicable way to the design of transition metal and nano-carbon composite catalysts for a broad application in the fields of energy chemistry.展开更多
Two-dimensional(2D)metal oxides and chalcogenides(MOs&MCs)have been regarded as a new class of promising electro-and photocatalysts for many important chemical reactions such as hydrogen evolution reaction,CO_(2) ...Two-dimensional(2D)metal oxides and chalcogenides(MOs&MCs)have been regarded as a new class of promising electro-and photocatalysts for many important chemical reactions such as hydrogen evolution reaction,CO_(2) reduction reaction and N2 reduction reaction in virtue of their outstanding physicochemical properties.However,pristine 2D MOs&MCs generally show the relatively poor catalytic performances due to the low electrical conductivity,few active sites and fast charge recombination.Therefore,considerable efforts have been devoted to engineering 2D MOs&MCs by rational structural design and chemical modification to further improve the catalytic activities.Herein,we comprehensively review the recent advances for engineering technologies of 2D MOs&MCs,which are mainly focused on the intercalation,doping,defects creation,facet design and compositing with functional materials.Meanwhile,the relationship between morphological,physicochemical,electronic,and optical properties of 2D MOs&MCs and their electro-and photocatalytic performances is also systematically discussed.Finally,we further give the prospect and challenge of the field and possible future research directions,aiming to inspire more research for achieving high-performance 2D MOs&MCs catalysts in energy storage and conversion fields.展开更多
The polysulfide shuttling and sluggish redox kinetics,due to the notorious adsorption-catalysis underperformance,are the ultimate obstacles of the practical application of lithium-sulfur(Li-S)batteries.Conventional ca...The polysulfide shuttling and sluggish redox kinetics,due to the notorious adsorption-catalysis underperformance,are the ultimate obstacles of the practical application of lithium-sulfur(Li-S)batteries.Conventional carbon-based and transition metal compound-based material solutions generally suffer from poor catalysis and adsorption,respectively,despite the performance gain in terms of the other.Herein,we have enhanced polysulfide adsorptioncatalytic capability and protected the Li anode using a complementary bimetallic carbide electrocatalyst,Co3 Mo3 C,modified commercial separator.With this demonstration,the potentials of bimetal compounds,which have been well recognized in other environmental catalysis,are also extended to Li-S batteries.Coupled with this modified separator,a simple cathode(S/Super P composite)can deliver high sulfur utilization,high rate performance,and excellent cycle stability with a low capacity decay rate of^0.034%per cycle at 1 C up to1000 cycles.Even at a high S-loading of 8.0 mg cm^-2 with electrolyte/sulfur ratio=6 m L g^-1,the cathode still exhibits high areal capacity of^6.8 m A h cm^-2.The experimental analysis and the first-principles calculations proved that the bimetallic carbide Co3 Mo3 C provides more binding sites for adsorbing polysulfides and catalyzing the multiphase conversion of sulfur/polysulfide/sulfide than monometallic carbide Mo2 C.Moreover,the modified separator can be reutilized with comparable electrochemical performance.We also showed other bimetallic carbides with similar catalytic effects on Li-S batteries and this material family has great promise indifferent energy electrocatalytic systems.展开更多
基金Project(20971041) supported by the National Natural Science Foundation of ChinaProject(09B032) supported by Scientific Research Fund of Hunan Provincial Education Department,China
文摘The sulfur phase in high sulfur-containing bauxite was studied by an X-ray diffraction analysis and a chemistry quantitative analysis.The methods for the removal of different shaped sulfur were also discussed.The results show that sulfur phases in high sulfur-containing bauxites exist in the main form of sulfide sulfur (pyrite) or sulfate sulfur,and the main sulfur forms of bauxites from different regions are not the same.Through a combination of an X-ray diffraction analysis and a chemistry quantitative analysis,the sulfur phases of high sulfur-containing bauxite could be accurately investigated.Deciding the main sulfur form of high sulfur-containing bauxite could provide theoretical instruction for choosing methods for the removal of sulfur from bauxite,and an oxidizing-roasting process is an effective way to remove sulfide sulfur from high sulfur-containing bauxite,the content of S^2-in crude ore in the digestion liquor is above 1.7 g/L,but in the roasted ore digestion liquor,it is below 0.18 g/L.Using the sodium carbonate solution washing technology to wash bauxite can effectively remove sulfate sulfur,the content of the total sulfur in ore is lowered to below 0.2% and can meet the production requirements for the sulfur content.
基金supported by Xiamen University Malaysia Research Fund (XMUMRF/2019-C3/IENG/0013)financial assistance and faculty start-up grants/supports from Xiamen University~~
文摘As one of the most appealing and attractive technologies, photocatalysis is widely used as a promising method to circumvent the environmental and energy problems. Due to its chemical stability and unique physicochemical, graphitic carbon nitride (g-C3N4) has become research hotspots in the community. However, g-C3N4 photocatalyst still suffers from many problems, resulting in unsatisfactory photocatalytic activity such as low specific surface area, high charge recombination and insufficient visible light utilization. Since 2009, g-C3N4-based heterostructures have attracted the attention of scientists worldwide for their greatly enhanced photocatalytic performance. Overall, this review summarizes the recent advances of g-C3N4-based nanocomposites modified with transition metal sulfide (TMS), including (1) preparation of pristine g-C3N4,(2) modification strategies of g-C3N4,(3) design principles of TMS-modified g-C3N4 heterostructured photocatalysts, and (4) applications in energy conversion. What is more, the characteristics and transfer mechanisms of each classification of the metal sulfide heterojunction system will be critically reviewed, spanning from the following categories:(1) Type I heterojunction,(2) Type II heterojunction,(3) p-n heterojunction,(4) Schottky junction and (5) Z-scheme heterojunction. Apart from that, the application of g-C3N4-based heterostructured photocatalysts in H2 evolution, CO2 reduction, N2 fixation and pollutant degradation will also be systematically presented. Last but not least, this review will conclude with invigorating perspectives, limitations and prospects for further advancing g-C3N4-based heterostructured photocatalysts toward practical benefits for a sustainable future.
文摘Expanding the optical absorption range of photocatalysts is still a key endeavor in graphitic carbon nitride(g-C_(3)N_(4))studies.Here,we report on a novel thiophene group extending the optical property,which is assigned to n-π^(*)electronic transitions involving the two lone pairs on sulfur(TLPS).The as-prepared samples,denoted as CN-ThAx(where x indicates the amount of ThA added,mg),showed an additional absorption above 500 nm as compared to pristine g-C_(3)N_(4).Further,the thiophene group enhanced charge carrier separation to suppress e‒/h+pair recombination.The experimental results suggest that the thiophene group can obstruct the polymerization of melem to generate a large plane,thus exposing the lone electron pairs on the sulfur.The photocatalytic activity was evaluated in the decomposition of bisphenol A and H2 evolution.Compared with g-C_(3)N_(4),the optimized CN-ThA_(30) sample led to a 6.6-and 2-fold enhancement of the degradation and H2 generation rates,respectively.The CN-ThA_(30) sample allowed for synchronous H2 production and BPA decomposition.
文摘Two-dimensional materials(2D)with unique physicochemical properties have been widely studied for their use in many applications,including as hydrogen evolution catalysts to improve the efficiency of water splitting.Recently,typical 2D materials MoS2,graphene,MXenes,and black phosphorus have been widely investigated for their application in the hydrogen evolution reaction(HER).In this review,we summarize three efficient strategies—defect engineering,heterostructure formation,and heteroatom doping—for improving the HER performance of 2D catalysts.The d-band theory,density of states,and Fermi energy level are discussed to provide guidance for the design and construction of novel 2D materials.The challenges and prospects of 2D materials in the HER are also considered.
基金Project(21007044) supported by the National Natural Science Foundation of ChinaProject(20050532009) supported by the Doctoral Foundation of Ministry of Education of China
文摘Activated carbon/nanosized CdS/chitosan(AC/n-CdS/CS) composites as adsorbent and photoactive catalyst were prepared under low temperature(≤60 ℃) and ambient pressure.Methyl orange(MO) was chosen as a model pollutant to evaluate synergistic effect of adsorption and photocatalytic decolorization by this innovative photocatalyst under visible light irradiation.Effects of various parameters such as catalyst amount,initial MO concentration,solution pH and reuse of catalyst on the decolorization of MO were investigated to optimize operational conditions.The decolorization of MO catalyzed by AC/n-CdS/CS fits the Langmuir-Hinshelwood kinetics model,and a surface reaction,where the dyes are absorbed,is the controlling step of the process.Decolorization efficiency of MO is improved with the increase in catalyst amount within a certain range.The photodecolorization of MO is more efficient in acidic media than alkaline media.The decolorization efficiency of MO is still higher than 84% after five cycles and 60 min under visible light irradiation,which confirms the reusability of AC/n-CdS/CS composite catalyst.
基金supported bythe National Natural Science Foundation of China under Grant No. 21307160the Natural Science Foundation of Shandong Province under Grant No. ZR2013EEQ030
文摘The denitrifying sulfide removal(DSR) process with bio-granules comprising both heterotrophic and autotrophic denitrifiers can simultaneously convert nitrate, sulfide and acetate species into di-nitrogen gas, elemental sulfur and carbon dioxide, respectively, at high loading rates. This study has determined that the reaction rate of sulfide oxidized into sulfur could be enhanced in the presence of 1,2-naphthoquinone-4-sulphonate(NQS). The presence of NQS mitigated the inhibition effects of sulfide species on denitrification. Furthermore, the reaction rates of nitrate and acetate to nitrogen gas and CO_2, respectively, were also promoted in the presence of NQS, thereby enhancing the performance of DSR granules. The advantages and disadvantages of applying the NQS-DSR process are discussed.
基金Supported by the National (863) Plan Fund Project China (2003AA33X100)
文摘There are sulfate and chloride ions corrosion and carbonation to concrete in coal mine. Based on taking test of accelerated carbonation, corrosion of 3.5% weight of NaCl solution and 5% weight of Na2SO4 solution of coal mine concretes, durability of con- cretes which include spray concrete of C20,high performance concretes of C30 and C50 and effect of fly ash on durability have been studied. Results suggest that the coal mineral high performance concretes show good resistance capacities of carbonation, sulfate and chloride corrosion to meet the coal mine construction. And the higher the strength grade is, the better the resistance capacity of corrosion of carbonation is, chloride and sulfate. Moreover, fly ash improves resistance capacity of high performance concrete(HPC) to chloride and sulfate but decreases the resistance capacity of C30’s to carbonation and average dynamic modulus.
文摘Reversible oxygen reaction plays a crucial role in rechargeable battery systems,but it is limited by the slow reaction kinetics.Herein,the ionic modulation of cobalt pentlandite coupled with nitrogen‐doped bowl‐like hollow carbon sphere is well designed on octahedral and tetrahedral sites.The robust FexCo9−xS8‐NHCS‐V with iron replacing at the octahedron possesses prolonged metal sulfur bond and exhibits excellent bifunctional electrocatalytic performance towards oxygen reduction reaction(ORR,E_(1/2)=0.80 V vs.RHE)and excellent oxygen evolution reaction(OER,E_(j=10)=1.53 V vs.RHE)in 0.1 mol/L KOH.Accordingly,a rechargeable Zn‐air battery of Fe_(x)Co_(9−x)S_(8)‐NHCS‐V cathode endows high energy efficiency(102 mW cm^(−2)),and a microbial fuel cell achieves a high‐power density(791±42 mW m^(−2)),outperforming the benchmark Pt/C catalyst.
基金the Foundation of Fellow of the Ministry of Education of China.
文摘The catalytic oxidization of CS2 over atmospheric particles and some oxide catalysts was explored through FT-IR, MS and a fixed-bed stainless steel reactor. The results show that atmospheric particles and some oxide catalysts exhibited considerable oxidizing activities for CS2 at ambient temperature. The reaction products are mainly COS and elemental sulfur, even CO2 on some catalysts. Among the catalysts, CaO has the strongest catalytic activity for oxidizing CS2. Fe2O3 is weaker than CaO. The catalytic activity for Al2O3 reduces considerably compared with the former two catalysts, and SiO2 the weakest. Atmospheric particle samples’ catalytic activity is between Fe2O3’s and Al2O3’s. The atmospheric particle sample collected mainly consists of Ca(Al2Si2O8) · 4H2O, which is also the main component of cement. COS, the main product, is formed by the catalytic oxidization of CS2 with adsorbed “molecular” oxygen over the catalysts’ surfaces. The concentration of adsorbed oxygen over catalysts’ surfaces may be the key factor contributed to the oxidizing activity. It is indicated that CS2 could be catalytically oxidized over atmospheric particles, which induced that this reaction may be another important source of atmospheric COS from CS2.
基金financially supported by the National Natural Science Foundation of China(21576056 and 21576057)Guangdong Natural Science Foundation(2017A030311016)+4 种基金Major Scientific Project of Guangdong University(2017KZDXM059)Science and Technology Research Project of Guangdong Province(2016A010103043)Science and Technology Research Project of Guangzhou(201607010232)Guangzhou University’s 2017 Training Program for Young Top-Notch Personnel(BJ201704)Australian Research Council(ARC)through Discovery Early Career Researcher Award(DE150101306)and Linkage Project(LP160100927)
文摘Hydrogen, serving as a clean, sustainable energy source, may be mainly produced from electrolysis water. Herein, we report cobalt disulphide encapsulated in self-catalyzed carbon nanotubes (S, N-CNTs/ CoS2@Co) serving as a bifunctional catalyst, which exhibits excellent hydrogen evolution reaction perfor-mance (10.0 mAcm^-2 at 0.112 V, and low Tafel slope for 104.9 mV dec^-1 ) and oxygen evolution reaction performance (10.0 mAcm^-2 at 1.57 V, and low Tafel slope for 76.1 mV dec^-1), meanwbile with a strong stability at various current densities. In-depth study reveals that the excellent catalytic properties can be mainly attributed to the increased catalytic sites induced by S, N co-doping, the improved electronic con-ductivity derived from the carbon nanotubes, and Mott-Schottky effect between the metal cobalt and semiconductive cobalt disulfide. Notably, when the bifunctional catalysts are applied to overall water splitting, a low potential of 1.633 V at the current density of 10.0 mAcm^-2 is achieved, which can com-pete with the precious metal catalyst benchmarks in alkaline media, demonstrating its promising prac-ticability in the realistic water splitting application. This work elucidates a practicable way to the design of transition metal and nano-carbon composite catalysts for a broad application in the fields of energy chemistry.
基金Australian Research Council(ARC)for funding received under the ARC Discovery Project scheme(DP180102752)the financial support via the ARC DECRA scheme(DE160100715)+1 种基金the support from the Shuguang Program supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(18SG035)State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,Donghua University(KF2015)。
文摘Two-dimensional(2D)metal oxides and chalcogenides(MOs&MCs)have been regarded as a new class of promising electro-and photocatalysts for many important chemical reactions such as hydrogen evolution reaction,CO_(2) reduction reaction and N2 reduction reaction in virtue of their outstanding physicochemical properties.However,pristine 2D MOs&MCs generally show the relatively poor catalytic performances due to the low electrical conductivity,few active sites and fast charge recombination.Therefore,considerable efforts have been devoted to engineering 2D MOs&MCs by rational structural design and chemical modification to further improve the catalytic activities.Herein,we comprehensively review the recent advances for engineering technologies of 2D MOs&MCs,which are mainly focused on the intercalation,doping,defects creation,facet design and compositing with functional materials.Meanwhile,the relationship between morphological,physicochemical,electronic,and optical properties of 2D MOs&MCs and their electro-and photocatalytic performances is also systematically discussed.Finally,we further give the prospect and challenge of the field and possible future research directions,aiming to inspire more research for achieving high-performance 2D MOs&MCs catalysts in energy storage and conversion fields.
基金supported by the National Natural Science Foundation of China(21863006,51662029,61974082 and 61704096)Youth Science Foundation of Jiangxi Province(20192BAB216001)Key Laboratory of Jiangxi Province for Environment and Energy Catalysis(20181BCD40004)。
文摘The polysulfide shuttling and sluggish redox kinetics,due to the notorious adsorption-catalysis underperformance,are the ultimate obstacles of the practical application of lithium-sulfur(Li-S)batteries.Conventional carbon-based and transition metal compound-based material solutions generally suffer from poor catalysis and adsorption,respectively,despite the performance gain in terms of the other.Herein,we have enhanced polysulfide adsorptioncatalytic capability and protected the Li anode using a complementary bimetallic carbide electrocatalyst,Co3 Mo3 C,modified commercial separator.With this demonstration,the potentials of bimetal compounds,which have been well recognized in other environmental catalysis,are also extended to Li-S batteries.Coupled with this modified separator,a simple cathode(S/Super P composite)can deliver high sulfur utilization,high rate performance,and excellent cycle stability with a low capacity decay rate of^0.034%per cycle at 1 C up to1000 cycles.Even at a high S-loading of 8.0 mg cm^-2 with electrolyte/sulfur ratio=6 m L g^-1,the cathode still exhibits high areal capacity of^6.8 m A h cm^-2.The experimental analysis and the first-principles calculations proved that the bimetallic carbide Co3 Mo3 C provides more binding sites for adsorbing polysulfides and catalyzing the multiphase conversion of sulfur/polysulfide/sulfide than monometallic carbide Mo2 C.Moreover,the modified separator can be reutilized with comparable electrochemical performance.We also showed other bimetallic carbides with similar catalytic effects on Li-S batteries and this material family has great promise indifferent energy electrocatalytic systems.