The interface is crucial for perovskite solar cells(PSCs).However,voids at interfaces induced by the trapped hygroscopic dimethyl sulfoxide(DMSO)can reduce charge extraction and accelerate the film degradation,serious...The interface is crucial for perovskite solar cells(PSCs).However,voids at interfaces induced by the trapped hygroscopic dimethyl sulfoxide(DMSO)can reduce charge extraction and accelerate the film degradation,seriously damaging the efficiency and stability.In this work,4,4’-dinonyl-2,2’-dipyridine(DN-DP),a Lewis base with long alkyl chains is introduced to solve this problem.Theoretical calculated and experimental results confirm that the dipyridyl group on DN-DP can more strongly coordinate with Pb^(2+)than that of the S=O group on DMSO.The strong coordination effect plays a crucial role in removing the DMSO-based adduct and reducing the formation of voids.Due to the electron-donating properties of pyridine,the existence of DN-DP in the perovskite film can passivate the defects and optimize the energy level alignment of the perovskite configuration.The open-circuit voltage(VOC)of the DN-DP-based PSC is improved from 1.107 V(control device)to 1.153 V,giving rise to a power conversion efficiency(PCE)of24.02%.Furthermore,benefiting from the moisture resistance stemming from the hydrophobic nonyl group,the PCE retains 90.4%of the initial performance after 1000 h of storage in the ambient condition.展开更多
Developing low-cost,efficient,and stable photocatalysts is one of the most promising methods for large-scale solar water splitting.As a metal-free semiconductor material with suitable band gap,graphitic carbon nitride...Developing low-cost,efficient,and stable photocatalysts is one of the most promising methods for large-scale solar water splitting.As a metal-free semiconductor material with suitable band gap,graphitic carbon nitride(g-C_(3)N_(4))has attracted attention in the field of photocatalysis,which is mainly attributed to its fascinating physicochemical and photoelectronic properties.However,several inherent limitations and shortcomings—involving high recombination rate of photocarriers,insufficient reaction kinetics,and optical absorption—impede the practical applicability of g-C_(3)N_(4).As an effective strategy,vacancy defect engineering has been widely used for breaking through the current limitations,considering its ability to optimize the electronic structure and surface morphology of g-C_(3)N_(4) to obtain the desired photocatalytic activity.This review summarizes the recent progress of vacancy defect engineered g-C_(3)N_(4) for solar water splitting.The fundamentals of solar water splitting with g-C_(3)N_(4) are discussed first.We then focus on the fabrication strategies and effect of vacancy generated in g-C_(3)N_(4).The advances of vacancy-modified g-C_(3)N_(4) photocatalysts toward solar water splitting are discussed next.Finally,the current challenges and future opportunities of vacancy-modified g-C_(3)N_(4) are summarized.This review aims to provide a theoretical basis and guidance for future research on the design and development of highly efficient defective g-C_(3)N_(4).展开更多
The electrochemical energy storage performance is greatly determined by the charge transfer and ion transportation occurring in the electrode materials.Therefore,the enhancement of electric conductivity and ionic mobi...The electrochemical energy storage performance is greatly determined by the charge transfer and ion transportation occurring in the electrode materials.Therefore,the enhancement of electric conductivity and ionic mobility is vital for high-performing and stable metal ion batteries.Here,we report the properties of oxygen vacancies(VO)and carbon co-doped TiO_(2) hollow spheres(HS-TiO_(2))and compared them with fully oxidized white TiO_(2) hollow spheres(W-TiO_(2)).Theoretical calculations and experimental results revealed that the introduction of carbon dopant and VO in anatase TiO_(2) reduced the bandgap and the existence of localized electrons,leading to a lower migration barrier of Li ions that promoted faster ion diffusion kinetics,enabling the HS-TiO_(2) with higher reversibility during the insertion and extraction of Li ions than the W-TiO_(2).This HS-TiO_(2) delivered superior lithium storage properties with a specific discharge capacity of 214.6 mAh g^(-1) for the 100th cycle at 200 mA g^(-1) and 116.3 mAh g^(-1) over 2000 cycles at a high rate of 2 A g^(-1).展开更多
The indiscriminate utilization of nondegradable polyethylene terephthalate(PET)-based products has triggered serious environmental pollution that has to be resolved vigorously.A simple synthesis of N-doped carbon nano...The indiscriminate utilization of nondegradable polyethylene terephthalate(PET)-based products has triggered serious environmental pollution that has to be resolved vigorously.A simple synthesis of N-doped carbon nanotubes from recycled PET(NCNTs_(r-PET))was developed by a nitric acid-assisted hydrothermal method.Experimental results and theoretical calculations show that the intrinsic defects in CNTs_(r-PET)would induce N-doping by NH_(3)generated from nitric acid during the hydrothermal process,thus producing the NCNTs_(r-PET).The life cycle assessment proves that the developed method for N-doped CNTs using r-PET as the carbon source is more environmentally friendly than the conventional chemical vapor deposition using acetylene as the carbon source.As a typical application,the NCNTs_(r-PET)delivered an impressive sodium storage capacity with an ultralong lifespan.This work not only provides a new route to upcycling waste plastics into valuable carbonaceous materials in an ecofriendly manner,but also reveals a basic understanding of the N-doping mechanism in carbonaceous materials.展开更多
基金supported by the National Key R&D Program of China(2019YFB1503200)the National Natural Science Foundation of China(52002105)+7 种基金the Key Research and Development Plan Project of Anhui Province(2022H11020014)the West Light Foundation of the Chinese Academy of Sciences(XAB2020YW11)the Collaborative Innovation Program of Hefei Science Center,CAS(2022HSC-CIP006)the Fundamental Research Funds for the Central Universities(JZ2021HGTB0105)the Hefei Institutes of Physical Science,Chinese Academy of Sciences Director’s Fund(YZJJ201902,YZJJZX202018)the Natural Science Foundation of Hebei Province(F2021208014)the Science and Technology Project of Hebei Education Department(QN2021063)the Science and Technology Research Project for the Colleges and Universities in Hebei Province(QN2022034)。
文摘The interface is crucial for perovskite solar cells(PSCs).However,voids at interfaces induced by the trapped hygroscopic dimethyl sulfoxide(DMSO)can reduce charge extraction and accelerate the film degradation,seriously damaging the efficiency and stability.In this work,4,4’-dinonyl-2,2’-dipyridine(DN-DP),a Lewis base with long alkyl chains is introduced to solve this problem.Theoretical calculated and experimental results confirm that the dipyridyl group on DN-DP can more strongly coordinate with Pb^(2+)than that of the S=O group on DMSO.The strong coordination effect plays a crucial role in removing the DMSO-based adduct and reducing the formation of voids.Due to the electron-donating properties of pyridine,the existence of DN-DP in the perovskite film can passivate the defects and optimize the energy level alignment of the perovskite configuration.The open-circuit voltage(VOC)of the DN-DP-based PSC is improved from 1.107 V(control device)to 1.153 V,giving rise to a power conversion efficiency(PCE)of24.02%.Furthermore,benefiting from the moisture resistance stemming from the hydrophobic nonyl group,the PCE retains 90.4%of the initial performance after 1000 h of storage in the ambient condition.
基金This work is supported mainly by the National Key Research and Development Program of China(Grant No.2018YFE0204000)the National Natural Science Foundation of China(Grant Nos.21975245,U20A20206,51972300,12004094,and 32101004)+4 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB43000000)the Science and Technology Research and Development Program of Handan(Grant No.21422111246)Prof.Y.Huang.also acknowledges the support from the Doctoral Special Fund Project of Hebei University of Engineering.Prof.K.Liu.appreciates the support from Youth Innovation Promotion Association,the Chinese Academy of Sciences(Grant No.2020114)the Beijing Nova Program(Grant No.2020117)Guangdong Basic and Applied Basic Research Foundation(Grant No.2022A1515110578).
文摘Developing low-cost,efficient,and stable photocatalysts is one of the most promising methods for large-scale solar water splitting.As a metal-free semiconductor material with suitable band gap,graphitic carbon nitride(g-C_(3)N_(4))has attracted attention in the field of photocatalysis,which is mainly attributed to its fascinating physicochemical and photoelectronic properties.However,several inherent limitations and shortcomings—involving high recombination rate of photocarriers,insufficient reaction kinetics,and optical absorption—impede the practical applicability of g-C_(3)N_(4).As an effective strategy,vacancy defect engineering has been widely used for breaking through the current limitations,considering its ability to optimize the electronic structure and surface morphology of g-C_(3)N_(4) to obtain the desired photocatalytic activity.This review summarizes the recent progress of vacancy defect engineered g-C_(3)N_(4) for solar water splitting.The fundamentals of solar water splitting with g-C_(3)N_(4) are discussed first.We then focus on the fabrication strategies and effect of vacancy generated in g-C_(3)N_(4).The advances of vacancy-modified g-C_(3)N_(4) photocatalysts toward solar water splitting are discussed next.Finally,the current challenges and future opportunities of vacancy-modified g-C_(3)N_(4) are summarized.This review aims to provide a theoretical basis and guidance for future research on the design and development of highly efficient defective g-C_(3)N_(4).
基金supported by the Hefei Institutes of Physical Science,the Chinese Academy of Sciences Director’s Fund(grant nos.YZJJ201902 and YZJJZX202018)the National Natural Science Foundation of China(grant no.52002105)+5 种基金the Key Research and Development Plan Project of Anhui Province(grant no.2022H11020014)the West Light Foundation of the Chinese Academy of Sciences(grant no.XAB2020YW11)the collaborative Innovation Program of Hefei Science Center,CAS(grant no.2022HSC-CIP006)the Natural Science Foundation of Hebei Province(grant no.F2021208014)the Science and Technology Project of Hebei Education Department(grant no.QN2021063)the Science and Technology Research Project for the Colleges and Universities in Hebei Province(grant no.QN2022034).
文摘The electrochemical energy storage performance is greatly determined by the charge transfer and ion transportation occurring in the electrode materials.Therefore,the enhancement of electric conductivity and ionic mobility is vital for high-performing and stable metal ion batteries.Here,we report the properties of oxygen vacancies(VO)and carbon co-doped TiO_(2) hollow spheres(HS-TiO_(2))and compared them with fully oxidized white TiO_(2) hollow spheres(W-TiO_(2)).Theoretical calculations and experimental results revealed that the introduction of carbon dopant and VO in anatase TiO_(2) reduced the bandgap and the existence of localized electrons,leading to a lower migration barrier of Li ions that promoted faster ion diffusion kinetics,enabling the HS-TiO_(2) with higher reversibility during the insertion and extraction of Li ions than the W-TiO_(2).This HS-TiO_(2) delivered superior lithium storage properties with a specific discharge capacity of 214.6 mAh g^(-1) for the 100th cycle at 200 mA g^(-1) and 116.3 mAh g^(-1) over 2000 cycles at a high rate of 2 A g^(-1).
基金National Natural Science Foundation of China,Grant/Award Numbers:22109023,22179022,22209027Industry-University-Research Joint Innovation Project of Fujian Province,Grant/Award Number:2021H6006+2 种基金FuXiaQuan National Independent Innovation Demonstration Zone Collaborative Innovation Platform,Grant/Award Number:2022-P-027Youth Innovation Fund of Fujian Province,Grant/Award Numbers:2021J05043,2022J05046Science and Technology。
文摘The indiscriminate utilization of nondegradable polyethylene terephthalate(PET)-based products has triggered serious environmental pollution that has to be resolved vigorously.A simple synthesis of N-doped carbon nanotubes from recycled PET(NCNTs_(r-PET))was developed by a nitric acid-assisted hydrothermal method.Experimental results and theoretical calculations show that the intrinsic defects in CNTs_(r-PET)would induce N-doping by NH_(3)generated from nitric acid during the hydrothermal process,thus producing the NCNTs_(r-PET).The life cycle assessment proves that the developed method for N-doped CNTs using r-PET as the carbon source is more environmentally friendly than the conventional chemical vapor deposition using acetylene as the carbon source.As a typical application,the NCNTs_(r-PET)delivered an impressive sodium storage capacity with an ultralong lifespan.This work not only provides a new route to upcycling waste plastics into valuable carbonaceous materials in an ecofriendly manner,but also reveals a basic understanding of the N-doping mechanism in carbonaceous materials.