The difficulty in fabricating a multifaceted composite heterojunction system based on Cd_(x) Zn_(1-x) S limits the enhancement of photocatalytic performance.In the present scrutiny,novel ZnO/Cd_(x) Zn_(1-x) S/CdS com-...The difficulty in fabricating a multifaceted composite heterojunction system based on Cd_(x) Zn_(1-x) S limits the enhancement of photocatalytic performance.In the present scrutiny,novel ZnO/Cd_(x) Zn_(1-x) S/CdS com-posite heterojunctions are successfully prepared by the alkaline dissolution etching method.The internal electric field at the interface of I-type and Z-scheme heterojunction improved the effective charge sepa-ration.The ZC 8 sample exhibits excellent photocatalytic performance and the H2 production efficiency is 15.67 mmol g^(−1) h^(−1) with good stability up to 82.9%in 24-hour cycles.The performance of CH_(4) and CO capacity in the CO_(2) RR process is 3.47μmol g^(−1) h^(−1) and 23.5μmol g^(−1) h^(−1),respectively.The photogener-ated accelerated charge transport is then examined in detail by in situ X-ray photoelectron spectroscopy(ISXPS)and density functional theory(DFT)calculations.This work presents a new idea for the synthe-sis of Cd_(x) Zn_(1-x) S solid-solution-based materials and provides a solid reference for the detailed mechanism regarding the electric field at the heterojunction interface.展开更多
Attempts to remove environmentally harmful materials in mass production industries are always a major issue and draw attention if the substitution guarantees a chance to lower fabrication cost and to improve device pe...Attempts to remove environmentally harmful materials in mass production industries are always a major issue and draw attention if the substitution guarantees a chance to lower fabrication cost and to improve device performance,as in a wide bandgap Zn_(1-x)Mg_(x)O(ZMO)to replace the CdS buffer in Cu(In_(1-x),Ga_(x))Se_(2)(CIGSe)thin-film solar cell structure.ZMO is one of the candidates for the buffer material in CIGSe thin-film solar cells with a wide and controllable bandgap depending on the Mg content,which can be helpful in attaining a suitable conduction band offset.Hence,compared to the fixed and limited bandgap of a CdS buffer,a ZMO buffer may provide advantages in V_(oc) and J_(sc) based on its controllable and wide bandgap,even with a relatively wider bandgap CIGSe thin-film solar cell.In addition,to solve problems with the defect sites at the ZMO/CIGSe junction interface,a few-nanometer ZnS layer is employed for heterojunction interface passivation,forming a ZMO/ZnS buffer structure by atomic layer deposition(ALD).Finally,a Cd-free all-dry-processed CIGSe solar cell with a wider bandgap(1.25 eV)and ALD-grown buffer structure exhibited the best power conversion efficiency of 19.1%,which exhibited a higher performance than the CdS counterpart.展开更多
Roman scattering measurement of （ 1 - x ） GeS2-x Ga2S3 system glasses was conducted in order to understand the microstructural change caused by the addition of Ga2S3 . According to the change of Raman spectra with t...Roman scattering measurement of （ 1 - x ） GeS2-x Ga2S3 system glasses was conducted in order to understand the microstructural change caused by the addition of Ga2S3 . According to the change of Raman spectra with the addition of Ga2S3, two main structural transformations were deduced ： the gradual enhancement of ethane- like structural units S3 Ge- GeS3 （ 250 cm ^- 1） and S3 Ga- GaS3 （270 cm ^- 1 ） and the appearance of charge imbalanced units [ Ga2 S2 （ S1/2 ）4 ]^2- and [Ga（ S1/2 ）4 ]^- . And this change of structural aspect seems to give as a clue to understanding the cause of the increased rare-earth solubility.展开更多
The global commitment to pivoting to sustainable energy and products calls for technology development to utilize solar energy for hydrogen(H_(2))and value-added chemicals production by biomass photoreforming.Herein,a ...The global commitment to pivoting to sustainable energy and products calls for technology development to utilize solar energy for hydrogen(H_(2))and value-added chemicals production by biomass photoreforming.Herein,a novel dual-functional marigold-like Zn_(x)Cd_(1-x)S homojunction has been the production of lactic acid with high-yield and H_(2)with high-efficiency by selective glucose photoreforming.The optimized Zn_(0.3)Cd_(0.7)S exhibits outstanding H_(2)generation(13.64 mmol h^(-1)g^(-1)),glucose conversion(96.40%),and lactic acid yield(76.80%),over 272.80 and 19.21 times higher than that of bare ZnS(0.05 mmol h^(-1)g^(-1))and CdS(0.71 mmol h^(-1)g^(-1))in H_(2)generation,respectively.The marigold-like morphology provides abundant active sites and sufficient substrates accessibility for the photocatalyst,while the specific role of the homojunction formed by hexagonal wurtzite(WZ)and cubic zinc blende(ZB)in photoreforming biomass has been demonstrated by density functional theory(DFT)calculations.Glucose is converted to lactic acid on the WZ surface of Zn_(0.3)Cd_(0.7)S via the photoactive species·O_(2)^(-),while the H_(2)is evolved from protons(H^(+))in H_(2)O on the ZB surface of Zn_(0.3)Cd_(0.7)S.This work paves a promising road for the production of sustainable energy and products by integrating photocatalysis and biorefine.展开更多
为降低Li_(1+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)电解质膜与锂金属负极之间的界面阻抗,抑制LATP与锂金属之间的副反应以及锂枝晶的生长,提高LATP电解质膜的性能,使用PVDF对LATP基电解质膜界面进行修饰,并研究其电化学性能。将LATP陶瓷...为降低Li_(1+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)电解质膜与锂金属负极之间的界面阻抗,抑制LATP与锂金属之间的副反应以及锂枝晶的生长,提高LATP电解质膜的性能,使用PVDF对LATP基电解质膜界面进行修饰,并研究其电化学性能。将LATP陶瓷粉末与聚氧化乙烯、LIFSI混合均匀后浇筑成膜,将PVDF溶液均匀涂覆在电解质膜表面,干燥得到修饰后的电解质膜。通过电化学实验、充放电实验、表面表征等方法,研究PVDF修饰后电解质膜的性能。结果显示,PVDF影响了LATP的晶体结构,优化了锂离子迁移通道。修饰后电解质膜的室温离子电导率提升,室温下电化学窗口由3.74 V增加到4.10 V,锂离子迁移数由0.915提升到0.978,组装锂金属对称电池在0.05 m A/cm^(2)电流密度下的循环时间从45 h提升到280 h以上,有效抑制了锂枝晶的生长,提升了电解质膜与锂金属界面稳定性。在电流密度0.025、0.050、0.100、0.200 m A/cm^(2)下的极化电压分别为27、60、110、220 m V。在LFP|SSCEs-1|Li全电池中循环超过25圈后形成了良好的SEI界面。从第25圈到第100圈容量保持率为87%,库仑效率始终保持在95%以上。PVDF修饰层提升了LATP电解质膜的电化学性能以及和锂金属界面的稳定性,对全固态锂电池的应用具有积极意义。展开更多
The achievement of chemical diversity and performance regulation of MAX phases primarily relies on solid solution approaches.However,the reported A-site solid solution is undervalued due to their expected chemical dis...The achievement of chemical diversity and performance regulation of MAX phases primarily relies on solid solution approaches.However,the reported A-site solid solution is undervalued due to their expected chemical disorder and compliance with Vegard’s law,as well as discontinuous composition and poor purity.Herein,we synthesized high-purity Ti_(2)(Sn_(x)Al_(1−x))C(x=0–1)solid solution by the feasible pressureless sintering,enabling us to investigate their property evolution upon the A-site composition.The formation mechanism of Ti_(2)(Sn_(x)Al_(1−x))C was revealed by thermal analysis,and crystal parameters were determined by Rietveld refinement of X-ray diffraction(XRD).The lattice constant(a)adheres to Vegard’s law,while the lattice constant(c)and internal free parameter(zM)have noticeable deviations from the law,which is caused by the significant nonlinear distortion of Ti_(6)C octahedron as Al atoms are substituted by Sn atoms.Also,the deviation also results in nonlinear changes in their physicochemical properties,which means that the solid solution often exhibits better performance than end members,such as hardness,electrical conductivity,and corrosion resistance.This work offers insights into the deviation from Vegard’s law observed in the A-site solid solution and indicates that the solid solution with enhanced performance may be obtained by tuning the A-site composition.展开更多
The replacement of liquid organic electrolytes with solid-state electrolytes(SSEs)is a feasible way to solve the safety issues and improve the energy density of lithium batteries.Developing SSEs materials that can wel...The replacement of liquid organic electrolytes with solid-state electrolytes(SSEs)is a feasible way to solve the safety issues and improve the energy density of lithium batteries.Developing SSEs materials that can well match with high-voltage cathodes and lithium metal anode is quite significant to develop high-energy-density lithium batteries.Li_(1+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)SSE with NASICON structure exhibits high ionic conductivity,low cost and superior air stability,which enable it as one of the most hopeful candidates for all-solidstate batteries(ASSBs).However,the high interfacial impedance between LATP and electrodes,and the severe interfacial side reactions with the lithium metal greatly limit its applications in ASSBs.This review introduces the crystal structure and ion transport mechanisms of LATP and summarizes the key factors affecting the ionic conductivity.The side reaction mechanisms of LATP with Li metal and the promising strategies for optimizing interfacial compatibility are reviewed.We also summarize the applications of LATP including as surface coatings of cathode particles,ion transport network additives and inorganic fillers of composite polymer electrolytes.At last,this review proposes the challenges and the future development directions of LATP in SSBs.展开更多
基金financially supported by the National Key Re-search and Development Program of China[No.2022YFF1202500,2022YFF1202502]the National Natural Science Foundation of China[62071459]+1 种基金the Subject arrangement Foundation of Shen-zhen[No.JCYJ20180507182057026]the International Science and Technology Cooperation Project of Bingtuan[No.2022BC008]。
文摘The difficulty in fabricating a multifaceted composite heterojunction system based on Cd_(x) Zn_(1-x) S limits the enhancement of photocatalytic performance.In the present scrutiny,novel ZnO/Cd_(x) Zn_(1-x) S/CdS com-posite heterojunctions are successfully prepared by the alkaline dissolution etching method.The internal electric field at the interface of I-type and Z-scheme heterojunction improved the effective charge sepa-ration.The ZC 8 sample exhibits excellent photocatalytic performance and the H2 production efficiency is 15.67 mmol g^(−1) h^(−1) with good stability up to 82.9%in 24-hour cycles.The performance of CH_(4) and CO capacity in the CO_(2) RR process is 3.47μmol g^(−1) h^(−1) and 23.5μmol g^(−1) h^(−1),respectively.The photogener-ated accelerated charge transport is then examined in detail by in situ X-ray photoelectron spectroscopy(ISXPS)and density functional theory(DFT)calculations.This work presents a new idea for the synthe-sis of Cd_(x) Zn_(1-x) S solid-solution-based materials and provides a solid reference for the detailed mechanism regarding the electric field at the heterojunction interface.
基金conducted under the framework of the research and development program of the Korea Institute of Energy Research(C4-2412 and C4-2413)supported by the National Research Foundation of Korea(grant number 2022M3J1A1063019)funded by the Ministry of Science and ICT.
文摘Attempts to remove environmentally harmful materials in mass production industries are always a major issue and draw attention if the substitution guarantees a chance to lower fabrication cost and to improve device performance,as in a wide bandgap Zn_(1-x)Mg_(x)O(ZMO)to replace the CdS buffer in Cu(In_(1-x),Ga_(x))Se_(2)(CIGSe)thin-film solar cell structure.ZMO is one of the candidates for the buffer material in CIGSe thin-film solar cells with a wide and controllable bandgap depending on the Mg content,which can be helpful in attaining a suitable conduction band offset.Hence,compared to the fixed and limited bandgap of a CdS buffer,a ZMO buffer may provide advantages in V_(oc) and J_(sc) based on its controllable and wide bandgap,even with a relatively wider bandgap CIGSe thin-film solar cell.In addition,to solve problems with the defect sites at the ZMO/CIGSe junction interface,a few-nanometer ZnS layer is employed for heterojunction interface passivation,forming a ZMO/ZnS buffer structure by atomic layer deposition(ALD).Finally,a Cd-free all-dry-processed CIGSe solar cell with a wider bandgap(1.25 eV)and ALD-grown buffer structure exhibited the best power conversion efficiency of 19.1%,which exhibited a higher performance than the CdS counterpart.
文摘Roman scattering measurement of （ 1 - x ） GeS2-x Ga2S3 system glasses was conducted in order to understand the microstructural change caused by the addition of Ga2S3 . According to the change of Raman spectra with the addition of Ga2S3, two main structural transformations were deduced ： the gradual enhancement of ethane- like structural units S3 Ge- GeS3 （ 250 cm ^- 1） and S3 Ga- GaS3 （270 cm ^- 1 ） and the appearance of charge imbalanced units [ Ga2 S2 （ S1/2 ）4 ]^2- and [Ga（ S1/2 ）4 ]^- . And this change of structural aspect seems to give as a clue to understanding the cause of the increased rare-earth solubility.
基金supported by the National Natural Science Foundation of China(No.32071713)the Outstanding Youth Foundation Project of Heilongjiang Province of China(JQ2019C001)。
文摘The global commitment to pivoting to sustainable energy and products calls for technology development to utilize solar energy for hydrogen(H_(2))and value-added chemicals production by biomass photoreforming.Herein,a novel dual-functional marigold-like Zn_(x)Cd_(1-x)S homojunction has been the production of lactic acid with high-yield and H_(2)with high-efficiency by selective glucose photoreforming.The optimized Zn_(0.3)Cd_(0.7)S exhibits outstanding H_(2)generation(13.64 mmol h^(-1)g^(-1)),glucose conversion(96.40%),and lactic acid yield(76.80%),over 272.80 and 19.21 times higher than that of bare ZnS(0.05 mmol h^(-1)g^(-1))and CdS(0.71 mmol h^(-1)g^(-1))in H_(2)generation,respectively.The marigold-like morphology provides abundant active sites and sufficient substrates accessibility for the photocatalyst,while the specific role of the homojunction formed by hexagonal wurtzite(WZ)and cubic zinc blende(ZB)in photoreforming biomass has been demonstrated by density functional theory(DFT)calculations.Glucose is converted to lactic acid on the WZ surface of Zn_(0.3)Cd_(0.7)S via the photoactive species·O_(2)^(-),while the H_(2)is evolved from protons(H^(+))in H_(2)O on the ZB surface of Zn_(0.3)Cd_(0.7)S.This work paves a promising road for the production of sustainable energy and products by integrating photocatalysis and biorefine.
文摘为降低Li_(1+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)电解质膜与锂金属负极之间的界面阻抗,抑制LATP与锂金属之间的副反应以及锂枝晶的生长,提高LATP电解质膜的性能,使用PVDF对LATP基电解质膜界面进行修饰,并研究其电化学性能。将LATP陶瓷粉末与聚氧化乙烯、LIFSI混合均匀后浇筑成膜,将PVDF溶液均匀涂覆在电解质膜表面,干燥得到修饰后的电解质膜。通过电化学实验、充放电实验、表面表征等方法,研究PVDF修饰后电解质膜的性能。结果显示,PVDF影响了LATP的晶体结构,优化了锂离子迁移通道。修饰后电解质膜的室温离子电导率提升,室温下电化学窗口由3.74 V增加到4.10 V,锂离子迁移数由0.915提升到0.978,组装锂金属对称电池在0.05 m A/cm^(2)电流密度下的循环时间从45 h提升到280 h以上,有效抑制了锂枝晶的生长,提升了电解质膜与锂金属界面稳定性。在电流密度0.025、0.050、0.100、0.200 m A/cm^(2)下的极化电压分别为27、60、110、220 m V。在LFP|SSCEs-1|Li全电池中循环超过25圈后形成了良好的SEI界面。从第25圈到第100圈容量保持率为87%,库仑效率始终保持在95%以上。PVDF修饰层提升了LATP电解质膜的电化学性能以及和锂金属界面的稳定性,对全固态锂电池的应用具有积极意义。
基金This work was financially supported by the National Natural Science Foundation of China(No.52171033)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX22_0247).
文摘The achievement of chemical diversity and performance regulation of MAX phases primarily relies on solid solution approaches.However,the reported A-site solid solution is undervalued due to their expected chemical disorder and compliance with Vegard’s law,as well as discontinuous composition and poor purity.Herein,we synthesized high-purity Ti_(2)(Sn_(x)Al_(1−x))C(x=0–1)solid solution by the feasible pressureless sintering,enabling us to investigate their property evolution upon the A-site composition.The formation mechanism of Ti_(2)(Sn_(x)Al_(1−x))C was revealed by thermal analysis,and crystal parameters were determined by Rietveld refinement of X-ray diffraction(XRD).The lattice constant(a)adheres to Vegard’s law,while the lattice constant(c)and internal free parameter(zM)have noticeable deviations from the law,which is caused by the significant nonlinear distortion of Ti_(6)C octahedron as Al atoms are substituted by Sn atoms.Also,the deviation also results in nonlinear changes in their physicochemical properties,which means that the solid solution often exhibits better performance than end members,such as hardness,electrical conductivity,and corrosion resistance.This work offers insights into the deviation from Vegard’s law observed in the A-site solid solution and indicates that the solid solution with enhanced performance may be obtained by tuning the A-site composition.
基金Key-Area Research and Development Program of Guangdong Province,Grant/Award Number:2020B090919001National Natural Science Foundation of China,Grant/Award Number:U2001220+1 种基金Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center,Grant/Award Number:XMHT20200203006Shenzhen Technical Plan Project,Grant/Award Number:JCYJ20180508152210821,JCYJ20170817161221958,JCYJ20180508152135822。
文摘The replacement of liquid organic electrolytes with solid-state electrolytes(SSEs)is a feasible way to solve the safety issues and improve the energy density of lithium batteries.Developing SSEs materials that can well match with high-voltage cathodes and lithium metal anode is quite significant to develop high-energy-density lithium batteries.Li_(1+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)SSE with NASICON structure exhibits high ionic conductivity,low cost and superior air stability,which enable it as one of the most hopeful candidates for all-solidstate batteries(ASSBs).However,the high interfacial impedance between LATP and electrodes,and the severe interfacial side reactions with the lithium metal greatly limit its applications in ASSBs.This review introduces the crystal structure and ion transport mechanisms of LATP and summarizes the key factors affecting the ionic conductivity.The side reaction mechanisms of LATP with Li metal and the promising strategies for optimizing interfacial compatibility are reviewed.We also summarize the applications of LATP including as surface coatings of cathode particles,ion transport network additives and inorganic fillers of composite polymer electrolytes.At last,this review proposes the challenges and the future development directions of LATP in SSBs.
