Commercial application of lithium-sulfur(Li-S) batteries is hindered by the insulating nature of sulfur and the dissolution of polysulfides. Here, a bioinspired 3D urchin-like N-doped Murray's carbon nanostructure...Commercial application of lithium-sulfur(Li-S) batteries is hindered by the insulating nature of sulfur and the dissolution of polysulfides. Here, a bioinspired 3D urchin-like N-doped Murray's carbon nanostructure(N-MCN) with interconnected micro-meso-macroporous structure and a polydopamine protection shell has been designed as an effective sulfur host for high-performance Li-S batteries. The advanced 3D hierarchically porous framework with the characteristics of the generalized Murray's law largely improves electrolyte diffusion, facilitates electrons/ions transfer and provides strong chemisorption for active species, leading to the synergistic structural and chemical confinement of polysulfides. As a result,the obtained P@S/N-MCN electrode with high areal sulfur loading demonstrates high capacity at high current densities after long cycles. This work reveals that following the generalized Murray's law is feasible to design high-performance sulfur cathode materials for potentially practical Li-S battery applications.展开更多
Lithium-sulfur batteries(LSBs) hold great potential for large-scale electrochemical energy storage applications. Currently, the shuttle of soluble lithium polysulfide(LiPSs) intermediates with sluggish conversion kine...Lithium-sulfur batteries(LSBs) hold great potential for large-scale electrochemical energy storage applications. Currently, the shuttle of soluble lithium polysulfide(LiPSs) intermediates with sluggish conversion kinetics and random deposition of Li2S have severely degraded the capacity, rate and cycling performances of LSBs, preventing their practical applications. In this work, ultrathin MoSe2 nanosheets with active edge sites were successfully grown on both internal and external surfaces of hollow carbon spheres with mesoporous walls(MCHS). The resulting MoSe2@MCHS composite acted as a novel functional reservoir for Li PSs with high chemical affinity and effectively mediated their fast redox conversion during charge/discharge as elucidated by experimental observations and first-principles density functional theory(DFT) calculations. The as-fabricated Li-S cells delivered high capacity, superior rate and excellent cyclability. The current work presents new insights on the delicate design and fabrication of novel functional composite electrode materials for rechargeable batteries with emerging applications.展开更多
Lithium-sulfur batteries(LSBs)are very promising for large-scale electrochemical energy storage.However,dissolution and shuttling of lithium polysulfides(LiPSs)intermediates have severely affected their overall electr...Lithium-sulfur batteries(LSBs)are very promising for large-scale electrochemical energy storage.However,dissolution and shuttling of lithium polysulfides(LiPSs)intermediates have severely affected their overall electrochemical properties and limited their practical application.Designing polar cathode hosts that can effectively bind LiPSs and simultaneously promote their redox conversion is crucial for realizing high-performance LSBs.Herein,we report bronze TiO2(TiO2-B)nanosheets(~5 nm in thickness)chemically bonded with carbon as a novel multifunctional cathode host for advanced LSBs.Experimental observation and first-principles density functional theory(DFT)calculations reveal that the TiO2-B with exposed(100)plane and Ti^3+ions exhibited high chemical affinity toward polysulfides and effectively confined them at surface.Meantime,Ti^3+ions and interface coupling with carbon promoted electronic conductivity of the composite cathode,leading to enhanced redox conversion kinetics of LiPSs during charge/discharge.Consequently,the as-assembled TiO2-B/S cathode manifested high capacity(1165 mAh/g at 0.2 C),excellent rate capability(244 mAh/g at 5 C)and outstanding cyclability(572 mAh/g over 500cycles at 0.2 C).This work sheds insights on rational design and fabrication of novel functional electrode materials for beyond Li-ion batteries.展开更多
Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions,Mn^(4+)ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices...Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions,Mn^(4+)ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices such as white light emitting diode(W-LED),plant cultivation LED,and temperature thermometer.Up to now,Mn^(4+)has been widely introduced into the lattices of various inorganic hosts for brightly redemitting phosphors.However,how to correlate the structure-activity relationship between host framework,luminescence property,and photoelectric device is urgently demanded.In this review,we thoroughly summarize the recent advances of Mn^(4+)doped phosphors.Meanwhile,several strategies like co-doping and defect passivation for improving Mn^(4+)emission are also discussed.Most importantly,the relationship between the protocols for tailoring the structures of Mn^(4+)doped phosphors,increased luminescence performance,and the targeted devices with efficient photoelectric and energy conversion efficiency is deeply correlated.Finally,the challenges and perspectives of Mn^(4+)doped phosphors for practical applications are anticipated.We cordially anticipate that this review can deliver a deep comprehension of not only Mn^(4+)luminescence mechanism but also the crystal structure tailoring strategy of phosphors,so as to spur innovative thoughts in designing advanced phosphors and deepening the applications.展开更多
Photocatalytic (PC) / Photoelectrochemical (PEC) water splitting under solar light irradiation is considered as a prospective technique to support the sustainable and renewable H_(2) economy and to reach the ultime go...Photocatalytic (PC) / Photoelectrochemical (PEC) water splitting under solar light irradiation is considered as a prospective technique to support the sustainable and renewable H_(2) economy and to reach the ultime goal of carbon neutral. TiO_(2) based photocatalysts with high chemical stability and excellent photocatalytic properties have great potential for solar-to-H_(2) conversion. To conquer the challenges of the large band-gap and rapid recombination of photo generated electron-holepairs in TiO_(2), non-metal doping turns out to be economic, facile, and effective on boosting the visible light activity. The localized defect states such as oxygen vacancy and Ti^(3+) generated by non-metal doping are located in the band-gap of TiO_(2), which result in the reduction of band-gap, thus a red-shift of the absorption edge. The hetero doping atoms such as B^(3+), I^(7+), S^(4+)/S^(6+), P^(5+) can also act as electron donors or trap sites which facilitate the charge carrier separation and suppress the recombination of electron-hole pairs. In this comprehensive review, we present the most recent advances on non-metal doped TiO_(2) photocatalysts in terms of fundamental aspects, origin of visible light activity and the PC / PEC behaviours for water splitting. In particular, the characteristics of different non-metal elements (N, C, B, S, P, Halogens) as dopants are discussed in details focusing on the synthesis approaches, characterization as well as the efficiency of PC and PEC water splitting. The present review aims at guiding the readers who want quick access to helpful information about how to efficiently improve the performance of photocatalysts by simple doping strategies and could stimulate new intuitive into the new doping strategies.展开更多
Lithium-selenium(Li-Se)battery has attracted growing attention.Nevertheless,its practical application is still impeded by the shuttle effect of the formed polyselenides.Herein,we report in-situ hydrothermal weaving th...Lithium-selenium(Li-Se)battery has attracted growing attention.Nevertheless,its practical application is still impeded by the shuttle effect of the formed polyselenides.Herein,we report in-situ hydrothermal weaving the three-dimensional(3 D)highly conductive hierarchically interconnected nanoporous web by threading microporous metal organic framework MIL-68(Al)crystals onto multi-walled carbon nanotubes(MWCNTs).Such 3 D hierarchically nanoporous web(3 D MIL-68(Al)@MWCNTs web)with a very high surface area,a large amount of micropores,electrical conductivity and elasticity strongly traps the soluble polyselenides during the electrochemical reaction and significantly facilitates lithium ion diffusion and electron transportation.Molecular dynamic calculation confirmed the strong affinity of MIL-68(Al)for the adsorption of polyselenides,quite suitable for Li-Se battery.Their hexahedral channels(1.56 nm)are more efficient for the confinement of polyselenides and for the diffusion of electrolytes compared to their smaller triangular channels(0.63 nm).All these excellent characteristics of 3 D MIL-68(Al)@MWCNTs web with suitable confinement of a large amount of selenium and the conductive linkage between MIL-68(Al)host by MWCNTs result in a high capacity of 453 m Ah/g at 0.2 C with 99.5%coulombic efficiency after 200 cycles with significantly improved cycle stability and rate performance.The 3 D MIL-68(Al)@MWCNTs web presents a good performance in Li-Se battery in term of the specific capacity and cycling stability and also in terms of rate performance compared with all the metal-organic framework(MOF)based or MOF derived porous carbons used in Li-Se battery.展开更多
Monolayer chemically converted graphene (CCG) nanosheets can be homogeneously self-assembled onto silicon wafer modified by 3-aminopropyl triethoxysilane (APTES) to form very thin graphene film. The CCG film was chara...Monolayer chemically converted graphene (CCG) nanosheets can be homogeneously self-assembled onto silicon wafer modified by 3-aminopropyl triethoxysilane (APTES) to form very thin graphene film. The CCG film was characterized by FT-IR, XRD, SEM, TEM and AFM. Results show that CCG sheets formed monolayer film after assembled onto silicon wafer and there is a very tight chemical bond between sheets and wafer. Furthermore, the electrical measurements revealed that the monolayer graphene film has an excellent electrical conductivity.展开更多
Graphitic carbon nitride(g-C_(3)N_(4))has attracted great interest in photocatalysis and photoelectrocatalysis.However,their poor hydrophilicity poses a great challenge for their applications in aqueous environment.He...Graphitic carbon nitride(g-C_(3)N_(4))has attracted great interest in photocatalysis and photoelectrocatalysis.However,their poor hydrophilicity poses a great challenge for their applications in aqueous environment.Here,we demonstrate synthesis of a hydrophilic bi-functional hierarchical architecture by the assembly of B-doped g-C_(3)N_(4)nanoplatelets.Such hierarchical B-doped g-C_(3)N_(4)material enables full utilization of their highly enhanced visible light absorption and photogenerated carrier separation in aqueous medium,leading to an excellent photocatalytic H_(2)O_(2)production rate of 4240.3μM g^(-1)h^(-1),2.84,2.64 and 2.13 times higher than that of the bulk g-C_(3)N_(4),g-C_(3)N_(4)nanoplatelets and bulk B doped g-C_(3)N_(4),respectively.Photoanodes based on these hierarchical architectures can generate an unprecedented photocurrent density of 1.72 m A cm^(-2)at 1.23 V under AM 1.5 G illumination for photoelectrochemical water splitting.This work makes a fundamental improvement towards large-scale exploitation of highly active,hydrophilic and stable metal-free g-C_(3)N_(4)photocatalysts for various practical applications.展开更多
Supercapacitor-like Na-ion batteries have attracted much attention due to the high energy density of batteries and power density of capacitors.Titanium dioxide(TiO_(2)),is a promising anode material.Its performance is...Supercapacitor-like Na-ion batteries have attracted much attention due to the high energy density of batteries and power density of capacitors.Titanium dioxide(TiO_(2)),is a promising anode material.Its performance is however seriously hindered by its low electrical conductivity and the sluggish diffusion of sodium ions(Na^(+))in the TiO_(2)matrix.Herein,this work combines porous TiO_(2)nanocubes with carbon nanotubes(CNTs)to enhance the electrical conductivity and accelerate Na^(+)diffusivity for Na-ion batteries(NIBs).In this composite,an interwoven scaffolded TiO_(2)/CNTs framework is formed to provide abundant channels and shorter diffusion pathways for electrons and ions.The in-situ X-ray diffraction and cyclic voltammetry confirm the low strain and superior transport kinetics in Na^(+)intercalation/extraction processes.In addition,the chemically bonded TiO_(2)/CNTs hybrid provides a more feasible channel for Na^(+)insertion/extraction with a much lower energy barrier.Consequently,the TiO_(2)/CNTs composite exhibits excellent electrochemical performance with a capacity of 223.4 m Ah g^(-1)at 1 C and a capacity of 142.8 m Ah g^(-1)at 10 C(3.35 A g^(-1)).The work here reveals that the combination of active materials with CNTs can largely improve the utilization efficiency and enhance their sodium storage.展开更多
Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three ...Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three dimensional ordered hierarchically porous carbon(3D OHPC) materials with micro/meso/macropores are designed and synthesized for Li-Se battery. The porous structure is tuned by following the concept of the generalized Murray’s law to facilitate the mass diffusion and reduce ion transport resistance.The optimized 3D Se/OHPC cathode exhibits a very high 2 nd discharge capacity of 651 m Ah/g and retains 361 m Ah/g after 200 cycles at 0.2 C. Even at a high current rate of 5 C, the battery still shows a discharge capacity as high as 155 m Ah/g. The improved electrochemical performance is attributed to the synergy effect of the interconnected and well-designed micro, meso and macroporosity while shortened ions diffusion pathways of such Murray materials accelerate its ionic and electronic conductivities leading to the enhanced electrochemical reaction. The diffusivity coefficient in Se/OHPC can reach a very high value of 1.3 × 10^(-11)cm^(2)/s, much higher than those in single pore size carbon hosts. Their effective volume expansion accommodation capability and reduced dissolution of polyselenides ensure the high stability of the battery. This work, for the first time, established the clear relationship between textural properties of cathode materials and their performance and demonstrates that the concept of the generalized Murray’s law can be used as efficient guidance for the rational design and synthesis of advanced hierarchically porous materials and the great potential of 3D OHPC materials as a practical high performance cathode material for Li-Se batteries.展开更多
The"one pot"simultaneous carbon coating and doping of TiO_(2) materials by the hydrolysis of TiCl4 in fructose is reported.The synergistic effect of carbon doping and coating of TiO_(2) to significantly boos...The"one pot"simultaneous carbon coating and doping of TiO_(2) materials by the hydrolysis of TiCl4 in fructose is reported.The synergistic effect of carbon doping and coating of TiO_(2) to significantly boost textural,optical and electronic properties and photocurrent of TiO_(2) for high performance visible light H2 production from water splitting has been comprehensively investigated.Carbon doping can significantly increase the thermal stability,thus inhibiting the phase transformation of the Titania material from anatase to rutile while carbon coating can suppress the grain aggregation of TiO_(2).The synergy of carbon doping and coating can not only ensure an enhanced narrowing effect of the electronic band gap of TiO_(2) thus extending the absorption of photocatalysts to the visible regions,but also promote dramatically the separation of electron-hole pairs.Owing to these synergistic effects,the carbon coated and doped TiO_(2) shows much superior photocatalytic activity for both degradation of organics and photocatalytic/photoelectro chemical(PEC)water splitting under simulated sunlight illumination.The photocatalytic activity of obtained materials can reach 5,4 and 2 times higher than that of pristine TiO_(2),carbon doped TiO_(2) and carbon coated TiO_(2),respectively in the degradation of organic pollutants.The carbon coated and doped TiO_(2) materials exhibited more than 37 times and hundreds of times photocurrent enhancement under simulated sunlight and visible light,respectively compared to that of pristine TiO_(2).The present work providing new comprehensive understanding on carbon coating and doping effect could be very helpful for the development of advanced TiO_(2) materials for a large series of applications.展开更多
Catalyst particle shapes and pore structure engineering are crucial for alleviating internal diffusion limitations in the hydrodesulfiirization(HDS)/hydrodeni-trogenation(HDN)of gas oil.The effects of catalyst particl...Catalyst particle shapes and pore structure engineering are crucial for alleviating internal diffusion limitations in the hydrodesulfiirization(HDS)/hydrodeni-trogenation(HDN)of gas oil.The effects of catalyst particle shapes(sphere,cylinder,trilobe,and tetralobe)and pore structures(pore diameter and porosity)on HDS/HDN performance at the particle scale are investigated via mathematical modeling.The relationship between particle shape and effectiveness factor is first established,and the specific surface areas of different catalyst particles show a positive correlation with the average HDS/HDN reaction rates.The catalyst particle shapes primarily alter the average HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor.An optimal average HDS/HDN reaction rate exists as the catalyst pore diameter and porosity increase,and this optimum value indicates a tradeoff between diffusion and reaction.In contrast to catalyst particle shapes,the catalyst pore diameter and the porosity of catalyst particles primarily alter the surface HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor.This study provides insights into the engineering of catalyst particle shapes and pore structures for improving HDS/HDN catalyst particle efficiency.展开更多
The introduction of vacancy defects in semiconductors has been proven to be a highly effective approach to improve their photocatalytic activity owing to their advantages of promoting light absorption,facilitating pho...The introduction of vacancy defects in semiconductors has been proven to be a highly effective approach to improve their photocatalytic activity owing to their advantages of promoting light absorption,facilitating photogenerated carrier separation,optimizing electronic structure,and enabling the production of reactive radicals.Herein,we outline the state-of-the-art vacancy-engineered photocatalysts in various applications and reveal how the vacancies influence photocatalytic performance.Specifically,the types of vacancy defects,the methods for tailoring vacancies,the advanced characteri-zation techniques,the categories of photocatalysts with vacancy defects,and the corresponding photocatalytic behaviors are presented.Meanwhile,the methods of vacancies creation and the related photocatalytic performance are correlated,which can be very useful to guide the readers to quickly obtain in-depth knowledge and to have a good idea about the selection of defect engineering methods.The precise characterization of vacancy defects is highly challenging.This review describes the accurate use of a series of characterization techniques with detailed comments and suggestions.This represents the uniqueness of this comprehensive review.The challenges and development prospects in engineering photocatalysts with vacancy defects for practical applications are discussed to provide a promising research direction in this field.展开更多
Owing to their facile reactants migration channels,large surface area,maximized exposure of reaction sites and efficient light utilization,three-dimensionally ordered macroporous(3DOM)materials have been extensively a...Owing to their facile reactants migration channels,large surface area,maximized exposure of reaction sites and efficient light utilization,three-dimensionally ordered macroporous(3DOM)materials have been extensively adopted in environmental fields such as pollutants removal,environmental detection as well as bacterial disinfection.In this review,the up-to-date 3DOM materials,the corresponding synthesis protocols and the related environmental applications involving photo/electrocatalytic pollutants decomposition,thermocatalytic volatile organic compounds(VOCs)elimination,hazardous substances sensing and bacteria inactivation are completely presented.Simultaneously,the inherent advantages and mechanisms of 3DOM materials in different environmental utilization are thoroughly demonstrated and summarized.Furthermore,the improved performance of environmental applications and the methods of fabricating 3DOM materials are correlated in depth,being favorable for readers to obtain the fundamental knowledge and to motivate some innovative thoughts for modifying 3DOM materials with further elevated environmental remediation capability.Finally,the current difficulties and prospects of 3DOM materials for large-scale and commercial applications are outlooked.This critical review is anticipated to promote the optimization of 3DOM materials and to ripen the related environmental remediation techniques.展开更多
Photocatalytic conversion of biomass is considered an effective,clean,and environmentally friendly route to obtain high-valued chemicals and hydrogen.However,the limited conversion efficiency and poor selectivity are ...Photocatalytic conversion of biomass is considered an effective,clean,and environmentally friendly route to obtain high-valued chemicals and hydrogen.However,the limited conversion efficiency and poor selectivity are still the main bottlenecks for photocatalytic biomass conversion.Herein,we report the highly selective photocatalytic conversion of glucose solution on holosymmetrically spherical three-dimensionally ordered macroporous TiO_(2)-CdSe heterojunction photonic crystal structure(s-TCS).The obtained s-TCS photocatalysts show excellent stability and strong light harvesting,uniform mass diffusion and exchange,and efficient photogenerated electrons/holes separation and utilization.The optimized s-TCS-4 photocatalyst displays the highest photocatalytic performance for glucose oxidation and hydrogen production.The glucose conversion,lactic acid selectivity,and yield on s-TCS-4 are about 95.9%,94.3%,and 96.4%,respectively.The photocatalytic production of lactic acid for s-TCS-4(18.5 g/L)is 2.3 times higher than the pure spherical TiO_(2) photonic crystal without CdSe(s-TiO_(2),8.1 g/L),and the hydrogen production rate of s-TCS-4 is 9.4 times that of s-TiO_(2).For the first time,we reveal that the photocatalytic conversion of glucose to lactic acid is a third-order and four-electron-involved reaction.This work could shed some new light on the efficient photocatalysis conversion of biomass to highly value-added products with high selectivity and yield,and simultaneously sustainable hydrogen evolution.展开更多
Electron donors are widely exploited in visible-light photocatalytic hydrogen production.As a typical electron donor pair and often the first choice for hydrogen production,the sodium sulfide-sodium sulfite pair has b...Electron donors are widely exploited in visible-light photocatalytic hydrogen production.As a typical electron donor pair and often the first choice for hydrogen production,the sodium sulfide-sodium sulfite pair has been extensively used.However,the resultant thiosulfate ions consume the photogenerated electrons to form an undesirable pseudocyclic electron transfer pathway during the photocatalytic process,strongly limiting the solar energy conversion efficiency.Here,we report novel and bioinspired electron donor pairs offering a noncyclic electron transfer pathway that provides more electrons without the consumption of the photogenerated electrons.Compared to the state-of-the-art electron donor pair Na_(2)S-Na_(2)SO_(3),these novel Na_(2)S-NaH_(2)PO_(2)and Na_(2)S-NaNO_(2)electron donor pairs enable an unprecedented enhancement of up to 370%and 140%for average photocatalytic H_(2)production over commercial CdS nanoparticles,and they are versatile for a large series of photocatalysts for visible-light water splitting.The discovery of these novel electron donor pairs can lead to a revolution in photocatalysis and is of great significance for industrial visible-light-driven H_(2)production.展开更多
基金financially supported by National Key Research and Development Program of China [2016YFA0202602, 2021YFE0115800]National Natural Science Foundation of China [22275142, U22B6011, U20A20122, 21671155]+4 种基金Program of Introducing Talents of Discipline to Universities-Plan 111 from the Ministry of Science and Technology and the Ministry of Education of China [Grant No. B20002]Sinopec Ministry of Science and Technology Basic Prospective Research Project [218025-9]Natural Science Foundation of Hubei Province [2021CFB082]Scientific Research Foundation of Wuhan Institute of Technology [K2021042]the Open Key Fund Project of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing [Wuhan University of Technology, 2022-KF-10]。
文摘Commercial application of lithium-sulfur(Li-S) batteries is hindered by the insulating nature of sulfur and the dissolution of polysulfides. Here, a bioinspired 3D urchin-like N-doped Murray's carbon nanostructure(N-MCN) with interconnected micro-meso-macroporous structure and a polydopamine protection shell has been designed as an effective sulfur host for high-performance Li-S batteries. The advanced 3D hierarchically porous framework with the characteristics of the generalized Murray's law largely improves electrolyte diffusion, facilitates electrons/ions transfer and provides strong chemisorption for active species, leading to the synergistic structural and chemical confinement of polysulfides. As a result,the obtained P@S/N-MCN electrode with high areal sulfur loading demonstrates high capacity at high current densities after long cycles. This work reveals that following the generalized Murray's law is feasible to design high-performance sulfur cathode materials for potentially practical Li-S battery applications.
基金financially supported by the National Natural Science Foundation of China (51302204, 21902122)Postdoctoral Science Foundation of China (2019M652723)+2 种基金Hunan Provincial Science and Technology Plan Project (No.2017TP1001)Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52)Hubei Provincial Department of Education for the “Chutian Scholar” program。
文摘Lithium-sulfur batteries(LSBs) hold great potential for large-scale electrochemical energy storage applications. Currently, the shuttle of soluble lithium polysulfide(LiPSs) intermediates with sluggish conversion kinetics and random deposition of Li2S have severely degraded the capacity, rate and cycling performances of LSBs, preventing their practical applications. In this work, ultrathin MoSe2 nanosheets with active edge sites were successfully grown on both internal and external surfaces of hollow carbon spheres with mesoporous walls(MCHS). The resulting MoSe2@MCHS composite acted as a novel functional reservoir for Li PSs with high chemical affinity and effectively mediated their fast redox conversion during charge/discharge as elucidated by experimental observations and first-principles density functional theory(DFT) calculations. The as-fabricated Li-S cells delivered high capacity, superior rate and excellent cyclability. The current work presents new insights on the delicate design and fabrication of novel functional composite electrode materials for rechargeable batteries with emerging applications.
基金financially supported by the National Natural Science Foundation of China(51302204,51672230,21902122)Postdoctoral Science Foundation of China(2019M652723)+2 种基金National Key R&D Program of China(2016YFA0202602)Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R52)the Hubei Provincial Department of Education for the“Chutian Scholar”program。
文摘Lithium-sulfur batteries(LSBs)are very promising for large-scale electrochemical energy storage.However,dissolution and shuttling of lithium polysulfides(LiPSs)intermediates have severely affected their overall electrochemical properties and limited their practical application.Designing polar cathode hosts that can effectively bind LiPSs and simultaneously promote their redox conversion is crucial for realizing high-performance LSBs.Herein,we report bronze TiO2(TiO2-B)nanosheets(~5 nm in thickness)chemically bonded with carbon as a novel multifunctional cathode host for advanced LSBs.Experimental observation and first-principles density functional theory(DFT)calculations reveal that the TiO2-B with exposed(100)plane and Ti^3+ions exhibited high chemical affinity toward polysulfides and effectively confined them at surface.Meantime,Ti^3+ions and interface coupling with carbon promoted electronic conductivity of the composite cathode,leading to enhanced redox conversion kinetics of LiPSs during charge/discharge.Consequently,the as-assembled TiO2-B/S cathode manifested high capacity(1165 mAh/g at 0.2 C),excellent rate capability(244 mAh/g at 5 C)and outstanding cyclability(572 mAh/g over 500cycles at 0.2 C).This work sheds insights on rational design and fabrication of novel functional electrode materials for beyond Li-ion batteries.
基金financially supported by the National Natural Science Foundation of China(52072101,51972088,U20A20122 and U1663225)the Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R52)of the Chinese Ministry of Education+2 种基金the Program of Introducing Talents of Discipline to Universities-Plan 111(Grant No.B20002)from the Ministry of Science and Technology and the Ministry of Education of ChinaHubei Provincial Department of Education for the“Chutian Scholar”programsupported by the European Commission Interreg V FranceWallonie-Vlaanderen project“Depollut Air”。
文摘Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions,Mn^(4+)ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices such as white light emitting diode(W-LED),plant cultivation LED,and temperature thermometer.Up to now,Mn^(4+)has been widely introduced into the lattices of various inorganic hosts for brightly redemitting phosphors.However,how to correlate the structure-activity relationship between host framework,luminescence property,and photoelectric device is urgently demanded.In this review,we thoroughly summarize the recent advances of Mn^(4+)doped phosphors.Meanwhile,several strategies like co-doping and defect passivation for improving Mn^(4+)emission are also discussed.Most importantly,the relationship between the protocols for tailoring the structures of Mn^(4+)doped phosphors,increased luminescence performance,and the targeted devices with efficient photoelectric and energy conversion efficiency is deeply correlated.Finally,the challenges and perspectives of Mn^(4+)doped phosphors for practical applications are anticipated.We cordially anticipate that this review can deliver a deep comprehension of not only Mn^(4+)luminescence mechanism but also the crystal structure tailoring strategy of phosphors,so as to spur innovative thoughts in designing advanced phosphors and deepening the applications.
基金supported by the National Natural Science Foundation of China(U1663225,21805280 and 21805220)the Youth Innovation Foundation of Xiamen City:3502Z20206085+4 种基金Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R52)The Opening Project of PCOSS,Xiamen University,201907the program of introducing Talents of discipline to Universities-111 Project(Grant No.B20002)the project“Depollut Air”of Interreg V France-Wallonie-Vlaanderenthe financial support from the China Scholarship Council(CSC)。
文摘Photocatalytic (PC) / Photoelectrochemical (PEC) water splitting under solar light irradiation is considered as a prospective technique to support the sustainable and renewable H_(2) economy and to reach the ultime goal of carbon neutral. TiO_(2) based photocatalysts with high chemical stability and excellent photocatalytic properties have great potential for solar-to-H_(2) conversion. To conquer the challenges of the large band-gap and rapid recombination of photo generated electron-holepairs in TiO_(2), non-metal doping turns out to be economic, facile, and effective on boosting the visible light activity. The localized defect states such as oxygen vacancy and Ti^(3+) generated by non-metal doping are located in the band-gap of TiO_(2), which result in the reduction of band-gap, thus a red-shift of the absorption edge. The hetero doping atoms such as B^(3+), I^(7+), S^(4+)/S^(6+), P^(5+) can also act as electron donors or trap sites which facilitate the charge carrier separation and suppress the recombination of electron-hole pairs. In this comprehensive review, we present the most recent advances on non-metal doped TiO_(2) photocatalysts in terms of fundamental aspects, origin of visible light activity and the PC / PEC behaviours for water splitting. In particular, the characteristics of different non-metal elements (N, C, B, S, P, Halogens) as dopants are discussed in details focusing on the synthesis approaches, characterization as well as the efficiency of PC and PEC water splitting. The present review aims at guiding the readers who want quick access to helpful information about how to efficiently improve the performance of photocatalysts by simple doping strategies and could stimulate new intuitive into the new doping strategies.
基金supported by the National Postdoctoral Program(2020M672782)National Natural Science Foundation of China(No.U1663225)+2 种基金Changjiang Scholars and Innovative Research Team in University(No.IRT15R52)National 111 project from the Ministry of Science and Technologythe Ministry of Education of China and the National Key R&D Program of China(No.2016YFA0202602)。
文摘Lithium-selenium(Li-Se)battery has attracted growing attention.Nevertheless,its practical application is still impeded by the shuttle effect of the formed polyselenides.Herein,we report in-situ hydrothermal weaving the three-dimensional(3 D)highly conductive hierarchically interconnected nanoporous web by threading microporous metal organic framework MIL-68(Al)crystals onto multi-walled carbon nanotubes(MWCNTs).Such 3 D hierarchically nanoporous web(3 D MIL-68(Al)@MWCNTs web)with a very high surface area,a large amount of micropores,electrical conductivity and elasticity strongly traps the soluble polyselenides during the electrochemical reaction and significantly facilitates lithium ion diffusion and electron transportation.Molecular dynamic calculation confirmed the strong affinity of MIL-68(Al)for the adsorption of polyselenides,quite suitable for Li-Se battery.Their hexahedral channels(1.56 nm)are more efficient for the confinement of polyselenides and for the diffusion of electrolytes compared to their smaller triangular channels(0.63 nm).All these excellent characteristics of 3 D MIL-68(Al)@MWCNTs web with suitable confinement of a large amount of selenium and the conductive linkage between MIL-68(Al)host by MWCNTs result in a high capacity of 453 m Ah/g at 0.2 C with 99.5%coulombic efficiency after 200 cycles with significantly improved cycle stability and rate performance.The 3 D MIL-68(Al)@MWCNTs web presents a good performance in Li-Se battery in term of the specific capacity and cycling stability and also in terms of rate performance compared with all the metal-organic framework(MOF)based or MOF derived porous carbons used in Li-Se battery.
基金a Chinese Ministry of Education "Changjiang" Innovative Research Team Program(IRT1169)"the Fundamental Research Funds for the Central Universities" (303-47110117,303-47110118,2012-yb-04,and 2012-Ia-008)+4 种基金NCET(NCET-11-0688)RFDP(20110143120006)NSFHB(2011CDB429)NFSC(51101115)Innovative Research Funds of SKLWUT(2011-la-024,2012-Ia-008,2011-PY-2,2011-PY-3)
文摘Monolayer chemically converted graphene (CCG) nanosheets can be homogeneously self-assembled onto silicon wafer modified by 3-aminopropyl triethoxysilane (APTES) to form very thin graphene film. The CCG film was characterized by FT-IR, XRD, SEM, TEM and AFM. Results show that CCG sheets formed monolayer film after assembled onto silicon wafer and there is a very tight chemical bond between sheets and wafer. Furthermore, the electrical measurements revealed that the monolayer graphene film has an excellent electrical conductivity.
基金financially supported by the National Natural Science Foundation of China(U1663225)the Changjiang Scholar Program of Chinese Ministry of Education(IRT15R52)the program of Introducing Talents of Discipline to Universities-Plan 111(B20002)of Ministry of Science and Technology and the Ministry of Education of China and the project “Depollut Air”of Interreg V France-WallonieVlaanderen。
文摘Graphitic carbon nitride(g-C_(3)N_(4))has attracted great interest in photocatalysis and photoelectrocatalysis.However,their poor hydrophilicity poses a great challenge for their applications in aqueous environment.Here,we demonstrate synthesis of a hydrophilic bi-functional hierarchical architecture by the assembly of B-doped g-C_(3)N_(4)nanoplatelets.Such hierarchical B-doped g-C_(3)N_(4)material enables full utilization of their highly enhanced visible light absorption and photogenerated carrier separation in aqueous medium,leading to an excellent photocatalytic H_(2)O_(2)production rate of 4240.3μM g^(-1)h^(-1),2.84,2.64 and 2.13 times higher than that of the bulk g-C_(3)N_(4),g-C_(3)N_(4)nanoplatelets and bulk B doped g-C_(3)N_(4),respectively.Photoanodes based on these hierarchical architectures can generate an unprecedented photocurrent density of 1.72 m A cm^(-2)at 1.23 V under AM 1.5 G illumination for photoelectrochemical water splitting.This work makes a fundamental improvement towards large-scale exploitation of highly active,hydrophilic and stable metal-free g-C_(3)N_(4)photocatalysts for various practical applications.
基金the financial support by the Bulgarian National Science Fund (Project FNI T02/4)the National Science Fund of Bulgaria for a financial support through Project E-01/07 2012
基金supported by the National Key R&D Program of China(2016YFA0202602,2016YFA0202603)the National Natural Science Foundation of China(U1663225)+1 种基金the 111 national project(Grant No.B20002)from Ministry of Science and Technologythe Ministry of Education and Sinopec Ministry of Science and Technology Basic Prospective Research Project(218025-9)。
文摘Supercapacitor-like Na-ion batteries have attracted much attention due to the high energy density of batteries and power density of capacitors.Titanium dioxide(TiO_(2)),is a promising anode material.Its performance is however seriously hindered by its low electrical conductivity and the sluggish diffusion of sodium ions(Na^(+))in the TiO_(2)matrix.Herein,this work combines porous TiO_(2)nanocubes with carbon nanotubes(CNTs)to enhance the electrical conductivity and accelerate Na^(+)diffusivity for Na-ion batteries(NIBs).In this composite,an interwoven scaffolded TiO_(2)/CNTs framework is formed to provide abundant channels and shorter diffusion pathways for electrons and ions.The in-situ X-ray diffraction and cyclic voltammetry confirm the low strain and superior transport kinetics in Na^(+)intercalation/extraction processes.In addition,the chemically bonded TiO_(2)/CNTs hybrid provides a more feasible channel for Na^(+)insertion/extraction with a much lower energy barrier.Consequently,the TiO_(2)/CNTs composite exhibits excellent electrochemical performance with a capacity of 223.4 m Ah g^(-1)at 1 C and a capacity of 142.8 m Ah g^(-1)at 10 C(3.35 A g^(-1)).The work here reveals that the combination of active materials with CNTs can largely improve the utilization efficiency and enhance their sodium storage.
基金financial support from the China Scholarship Council (CSC) and a scholarship from the Laboratory of Inorganic Materials Chemistry,Universitéde Namur,Belgiumfinancially supported by the National Postdoctoral Program (Grant No. 2020M672782)+2 种基金the National Natural Science Foundation of China (Grant No. U1663225)the the Program of Introducing Talents of Discipline to Universities-National 111 Project from the Ministry of Science and Technology and the Ministry of Education of China (Grant No. B20002)the National Key R&D Program of China (Grant No. 2016YFA0202602)。
文摘Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three dimensional ordered hierarchically porous carbon(3D OHPC) materials with micro/meso/macropores are designed and synthesized for Li-Se battery. The porous structure is tuned by following the concept of the generalized Murray’s law to facilitate the mass diffusion and reduce ion transport resistance.The optimized 3D Se/OHPC cathode exhibits a very high 2 nd discharge capacity of 651 m Ah/g and retains 361 m Ah/g after 200 cycles at 0.2 C. Even at a high current rate of 5 C, the battery still shows a discharge capacity as high as 155 m Ah/g. The improved electrochemical performance is attributed to the synergy effect of the interconnected and well-designed micro, meso and macroporosity while shortened ions diffusion pathways of such Murray materials accelerate its ionic and electronic conductivities leading to the enhanced electrochemical reaction. The diffusivity coefficient in Se/OHPC can reach a very high value of 1.3 × 10^(-11)cm^(2)/s, much higher than those in single pore size carbon hosts. Their effective volume expansion accommodation capability and reduced dissolution of polyselenides ensure the high stability of the battery. This work, for the first time, established the clear relationship between textural properties of cathode materials and their performance and demonstrates that the concept of the generalized Murray’s law can be used as efficient guidance for the rational design and synthesis of advanced hierarchically porous materials and the great potential of 3D OHPC materials as a practical high performance cathode material for Li-Se batteries.
基金supported by the National Natural Science Foundation of China(U1663225,21805280)Program for Changjiang Scholars and Innovative Research Team in University(IRT15R52)+2 种基金the Minstry of Education of Chinathe 111 Project(Grant No.B20002)from the Ministry of Science and Technology and the Ministry of Education of China,China,European Commission,Interreg V France-Wallonie-Vlaanderen(Depollutair)the Fundamental Research Funds for the Central Universities(WUT:2017III001),Chinathe FJIRSM&IUE Joint Research Fund(RHZX-2018-002),China for supporting this work。
文摘The"one pot"simultaneous carbon coating and doping of TiO_(2) materials by the hydrolysis of TiCl4 in fructose is reported.The synergistic effect of carbon doping and coating of TiO_(2) to significantly boost textural,optical and electronic properties and photocurrent of TiO_(2) for high performance visible light H2 production from water splitting has been comprehensively investigated.Carbon doping can significantly increase the thermal stability,thus inhibiting the phase transformation of the Titania material from anatase to rutile while carbon coating can suppress the grain aggregation of TiO_(2).The synergy of carbon doping and coating can not only ensure an enhanced narrowing effect of the electronic band gap of TiO_(2) thus extending the absorption of photocatalysts to the visible regions,but also promote dramatically the separation of electron-hole pairs.Owing to these synergistic effects,the carbon coated and doped TiO_(2) shows much superior photocatalytic activity for both degradation of organics and photocatalytic/photoelectro chemical(PEC)water splitting under simulated sunlight illumination.The photocatalytic activity of obtained materials can reach 5,4 and 2 times higher than that of pristine TiO_(2),carbon doped TiO_(2) and carbon coated TiO_(2),respectively in the degradation of organic pollutants.The carbon coated and doped TiO_(2) materials exhibited more than 37 times and hundreds of times photocurrent enhancement under simulated sunlight and visible light,respectively compared to that of pristine TiO_(2).The present work providing new comprehensive understanding on carbon coating and doping effect could be very helpful for the development of advanced TiO_(2) materials for a large series of applications.
基金the National Natural Science Foundation of China(Grant Nos.22038003,21922803,22178100 and 21776077)the Innovation Program of Shanghai Municipal Education Commission,the Program of Shanghai Academic/Technology Research Leader(Grant No.21XD1421000).
文摘Catalyst particle shapes and pore structure engineering are crucial for alleviating internal diffusion limitations in the hydrodesulfiirization(HDS)/hydrodeni-trogenation(HDN)of gas oil.The effects of catalyst particle shapes(sphere,cylinder,trilobe,and tetralobe)and pore structures(pore diameter and porosity)on HDS/HDN performance at the particle scale are investigated via mathematical modeling.The relationship between particle shape and effectiveness factor is first established,and the specific surface areas of different catalyst particles show a positive correlation with the average HDS/HDN reaction rates.The catalyst particle shapes primarily alter the average HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor.An optimal average HDS/HDN reaction rate exists as the catalyst pore diameter and porosity increase,and this optimum value indicates a tradeoff between diffusion and reaction.In contrast to catalyst particle shapes,the catalyst pore diameter and the porosity of catalyst particles primarily alter the surface HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor.This study provides insights into the engineering of catalyst particle shapes and pore structures for improving HDS/HDN catalyst particle efficiency.
基金This study was also supported by the European Commission Interreg V France-Wallonie-Vlaanderen project“DepollutAir.”Yang Ding is grateful for the financial support of the China Scholarship Council(201808310127)This study was financially supported by the National Natural Science Foundation of China(U20A20122)+1 种基金the Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R52)of the Chinese Ministry of Education,the Program of Introducing Talents of Discipline to Universities-Plan 111(Grant No.B20002)the Ministry of Science and Technology and the Ministry of Education of China,and the National Key R&D Program of China(2016YFA0202602).
文摘The introduction of vacancy defects in semiconductors has been proven to be a highly effective approach to improve their photocatalytic activity owing to their advantages of promoting light absorption,facilitating photogenerated carrier separation,optimizing electronic structure,and enabling the production of reactive radicals.Herein,we outline the state-of-the-art vacancy-engineered photocatalysts in various applications and reveal how the vacancies influence photocatalytic performance.Specifically,the types of vacancy defects,the methods for tailoring vacancies,the advanced characteri-zation techniques,the categories of photocatalysts with vacancy defects,and the corresponding photocatalytic behaviors are presented.Meanwhile,the methods of vacancies creation and the related photocatalytic performance are correlated,which can be very useful to guide the readers to quickly obtain in-depth knowledge and to have a good idea about the selection of defect engineering methods.The precise characterization of vacancy defects is highly challenging.This review describes the accurate use of a series of characterization techniques with detailed comments and suggestions.This represents the uniqueness of this comprehensive review.The challenges and development prospects in engineering photocatalysts with vacancy defects for practical applications are discussed to provide a promising research direction in this field.
基金supported by the National Natural Science Foundation of China(22293022,U20A20122)the Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R52)of the Chinese Ministry of Education+2 种基金the Program of Introducing Talents of Discipline to Universities-Plan 111(B20002)from the Ministry of Science and Technology and the Ministry of Education of Chinasupported by the European Commission Interreg V France-Wallonie-Vlaanderen project“Depollut Air”the Hubei Provincial Department of Education for the“Chutian Scholar”Program
文摘Owing to their facile reactants migration channels,large surface area,maximized exposure of reaction sites and efficient light utilization,three-dimensionally ordered macroporous(3DOM)materials have been extensively adopted in environmental fields such as pollutants removal,environmental detection as well as bacterial disinfection.In this review,the up-to-date 3DOM materials,the corresponding synthesis protocols and the related environmental applications involving photo/electrocatalytic pollutants decomposition,thermocatalytic volatile organic compounds(VOCs)elimination,hazardous substances sensing and bacteria inactivation are completely presented.Simultaneously,the inherent advantages and mechanisms of 3DOM materials in different environmental utilization are thoroughly demonstrated and summarized.Furthermore,the improved performance of environmental applications and the methods of fabricating 3DOM materials are correlated in depth,being favorable for readers to obtain the fundamental knowledge and to motivate some innovative thoughts for modifying 3DOM materials with further elevated environmental remediation capability.Finally,the current difficulties and prospects of 3DOM materials for large-scale and commercial applications are outlooked.This critical review is anticipated to promote the optimization of 3DOM materials and to ripen the related environmental remediation techniques.
基金supported by the National Key R&D Program of China(grant nos.2016YFA0202602 and 2021YFE0115800)National Natural Science Foundation of China(grant nos.21805220,U20A20122,and 52103285)+3 种基金Program of Introducing Talents of Discipline to Universities-Plan 111 from the Ministry of Science and Technology and the Ministry of Education of China(grant no.B20002)Natural Science Foundation of Hubei Province(grant nos.2020CFB416,2018CFB242,and 2018CFA054)the Fundamental Research Funds for the Central Universities(WUT:grant no.2021III016GX)Youth Innovation Research Fund project and the Open Fund Project of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing。
文摘Photocatalytic conversion of biomass is considered an effective,clean,and environmentally friendly route to obtain high-valued chemicals and hydrogen.However,the limited conversion efficiency and poor selectivity are still the main bottlenecks for photocatalytic biomass conversion.Herein,we report the highly selective photocatalytic conversion of glucose solution on holosymmetrically spherical three-dimensionally ordered macroporous TiO_(2)-CdSe heterojunction photonic crystal structure(s-TCS).The obtained s-TCS photocatalysts show excellent stability and strong light harvesting,uniform mass diffusion and exchange,and efficient photogenerated electrons/holes separation and utilization.The optimized s-TCS-4 photocatalyst displays the highest photocatalytic performance for glucose oxidation and hydrogen production.The glucose conversion,lactic acid selectivity,and yield on s-TCS-4 are about 95.9%,94.3%,and 96.4%,respectively.The photocatalytic production of lactic acid for s-TCS-4(18.5 g/L)is 2.3 times higher than the pure spherical TiO_(2) photonic crystal without CdSe(s-TiO_(2),8.1 g/L),and the hydrogen production rate of s-TCS-4 is 9.4 times that of s-TiO_(2).For the first time,we reveal that the photocatalytic conversion of glucose to lactic acid is a third-order and four-electron-involved reaction.This work could shed some new light on the efficient photocatalysis conversion of biomass to highly value-added products with high selectivity and yield,and simultaneously sustainable hydrogen evolution.
基金This work is financially supported by the National Key R&D Program of China(grant nos.2016YFA0202602 and 2021YFE0115800)the National Natural Science Foundation of China(grant nos.U20A20122 and 52103285)+3 种基金the Program of Introducing Talents of Discipline to Universities-Plan 111 from the Ministry of Science and Technology and the Ministry of Education of China(grant no.B20002)the“Algae Factory”European Horizon 2020 Program financed by FEDER and Wallonia Region of Belgium(grant no.1610187)the“DepollutAir”of Interreg V France-Wallonie-Vlaanderen and the Natural Science Foundation of Hubei Province(grant nos.2018CFB242 and 2020CFB416)the Youth Innovation Research Fund Project of the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing.T.H.acknowledges support from the Royal Academy of Engineering through a Research Fellowship(Graphlex).We also thank Prof.Pierre Van Cutsem,Department of Biology,University of Namur for his advice.
文摘Electron donors are widely exploited in visible-light photocatalytic hydrogen production.As a typical electron donor pair and often the first choice for hydrogen production,the sodium sulfide-sodium sulfite pair has been extensively used.However,the resultant thiosulfate ions consume the photogenerated electrons to form an undesirable pseudocyclic electron transfer pathway during the photocatalytic process,strongly limiting the solar energy conversion efficiency.Here,we report novel and bioinspired electron donor pairs offering a noncyclic electron transfer pathway that provides more electrons without the consumption of the photogenerated electrons.Compared to the state-of-the-art electron donor pair Na_(2)S-Na_(2)SO_(3),these novel Na_(2)S-NaH_(2)PO_(2)and Na_(2)S-NaNO_(2)electron donor pairs enable an unprecedented enhancement of up to 370%and 140%for average photocatalytic H_(2)production over commercial CdS nanoparticles,and they are versatile for a large series of photocatalysts for visible-light water splitting.The discovery of these novel electron donor pairs can lead to a revolution in photocatalysis and is of great significance for industrial visible-light-driven H_(2)production.
