Graphitic carbon nitride(g-C_(3)N_(4))has been extensively doped with alkali metals to enlarge photocatalytic output,in which cesium(Cs)doping is predicted to be the most efficient.Nevertheless,the sluggish diffusion ...Graphitic carbon nitride(g-C_(3)N_(4))has been extensively doped with alkali metals to enlarge photocatalytic output,in which cesium(Cs)doping is predicted to be the most efficient.Nevertheless,the sluggish diffusion and doping kinetics of precursors with high melting points,along with imprecise regulation,have raised the debate on whether Cs doping could make sense.For this matter,we attempt to confirm the positive effects of Cs doping on multifunctional photocatalysis by first using cesium acetate with the character of easy manipulation.The optimized Csdoped g-C_(3)N_(4)(CCN)shows a 41.6-fold increase in visible-light-driven hydrogen evolution reaction(HER)compared to pure g-C_(3)N_(4) and impressive degradation capability,especially with 77%refractory tetracycline and almost 100%rhodamine B degradedwithin an hour.The penetration ofCs+is demonstrated to be a mode of interlayer doping,and Cs–N bonds(especially with sp^(2) pyridine N in C═N–C),along with robust chemical interaction and electron exchange,are fabricated.This atomic configuration triggers the broadened spectral response,the improved charge migration,and the activated photocatalytic capacity.Furthermore,we evaluate the CCN/cadmium sulfide hybrid as a Z-scheme configuration,promoting the visible HER yield to 9.02 mmol g^(−1) h^(−1),which is the highest ever reported among all CCN systems.This work adds to the rapidly expanding field of manipulation strategies and supports further development of mediating served for photocatalysis.展开更多
Nowadays, the soar of photovoltaic performance of perovskite solar cells has set off a fever in the study of metal halide perovskite materials. The excellent optoelectronic properties and defect tolerance feature allo...Nowadays, the soar of photovoltaic performance of perovskite solar cells has set off a fever in the study of metal halide perovskite materials. The excellent optoelectronic properties and defect tolerance feature allow metal halide perovskite to be employed in a wide variety of applications. This article provides a holistic review over the current progress and future prospects of metal halide perovskite materials in representative promising applications, including traditional optoelectronic devices(solar cells, light-emitting diodes, photodetectors, lasers), and cutting-edge technologies in terms of neuromorphic devices(artificial synapses and memristors) and pressure-induced emission. This review highlights the fundamentals, the current progress and the remaining challenges for each application, aiming to provide a comprehensive overview of the development status and a navigation of future research for metal halide perovskite materials and devices.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
In organic solar cells,the singlet and triplet excitons dissociate into free charge carriers with different mechanisms due to their opposite spin state.Therefore,the ratio of the singlet and triplet excitons directly ...In organic solar cells,the singlet and triplet excitons dissociate into free charge carriers with different mechanisms due to their opposite spin state.Therefore,the ratio of the singlet and triplet excitons directly affects the photocurrent.Many methods were used to optimize the performance of the low-efficiency solar cell by improving the ratio of triplet excitons,which shows a long diffusion length.Here we observed that in high-efficiency systems,the proportion of singlet excitons under linearly polarized light excitation is higher than that of circularly polarized light.Since the singlet charge transfer state has lower binding energy than the triplet state,it makes a significant contribution to the charge carrier generation and enhancement of the photocurrent.Further,the positive magnetic field effect reflects that singlet excitons dissociation plays a major role in the photocurrent,which is opposite to the case of low-efficiency devices where triplet excitons dominate the photocurrent.展开更多
Optical frequency combs(OFCs)have great potential in communications,especially in dense wavelength-division multiplexing.However,the size of traditional OFCs based on conventional optical microcavities or dispersion f...Optical frequency combs(OFCs)have great potential in communications,especially in dense wavelength-division multiplexing.However,the size of traditional OFCs based on conventional optical microcavities or dispersion fibers is at least tens of micrometers,far larger than that of nanoscale electronic chips.Therefore,reducing the size of OFCs to match electronic chips is of necessity.Here,for the first time to our knowledge,we introduce surface plasmon polaritons(SPPs)to the construction of OFCs to realize a miniature device.The thickness of our device is reduced below 1μm.Though the presence of SPPs may induce ohmic and scattering loss,the threshold of the device is obtained as 9μW,comparable to the conventional device.Interestingly,the response time is 13.2 ps,much faster than the optical counterparts.This work provides a feasible strategy for the miniaturization of OFCs.展开更多
Earthworms have the ability to accumulate of heavy metals, however, there was few studies that addressed the metals in earthworm at subcellular levels in fields. The distributions of metals (Cd, Cu, Zn, and Pb) in s...Earthworms have the ability to accumulate of heavy metals, however, there was few studies that addressed the metals in earthworm at subcellular levels in fields. The distributions of metals (Cd, Cu, Zn, and Pb) in subcellular fractions (cytosol, debris, and granules) of earthworm Metaphire californica were investigated. The relationship between soil metals and earthworms were analyzed to explain its high plasticity to inhabit in situ contaminated soil of Hunan Province, south China. The concentration of Cd in subcellular compartments showed the same pattern as Cu in the order of cytosol 〉 debris 〉 granules. The distribution of Zn and Pb in earthworms indicated a similar propensity for different subcellular fractions that ranked as granules 〉 debris 〉 cytosol for Zn, and granules 〉 cytosol 〉 debris for Pb. The internal metal concentrations in earthworms increased with the soil metals (p 〈 0.05). Significant positive correlations were found between soil Cd and Cd concentrations in cytosol and debris (p 〈 0.01). Moreover, the soil Pb concentration significantly influenced the Pb concentrations in cytosol and debris (p 〈 0.01), similar to that of Cd. The soil Cu concentrations was only associated with the Cu in granules (p 〈 0.05). Soil Zn concentrations correlated with the Zn concentrations in each subcellular fraction (p 〈 0.05). Our results provide insights into the variations of metals partitioning in earthworms at subcellular levels and the relationships of soil metals, which could be one of the detoxiflcation strategies to adapt the long-term contaminated environment.展开更多
基金supported primarily by the National Natural Science Foundation of China(Contract No.21975245,51972300,62274155,and U20A20206)the National Key Research and Development Program of China(Grant No.2018YFE0204000)+2 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB43000000)the National Natural Science Foundation of China under Grant No.62175231.Prof.Kong Liu appreciates the support from the Youth Innovation Promotion Association,the Chinese Academy of Sciences(No.2020114)the Beijing Nova Program(No.2020117).
文摘Graphitic carbon nitride(g-C_(3)N_(4))has been extensively doped with alkali metals to enlarge photocatalytic output,in which cesium(Cs)doping is predicted to be the most efficient.Nevertheless,the sluggish diffusion and doping kinetics of precursors with high melting points,along with imprecise regulation,have raised the debate on whether Cs doping could make sense.For this matter,we attempt to confirm the positive effects of Cs doping on multifunctional photocatalysis by first using cesium acetate with the character of easy manipulation.The optimized Csdoped g-C_(3)N_(4)(CCN)shows a 41.6-fold increase in visible-light-driven hydrogen evolution reaction(HER)compared to pure g-C_(3)N_(4) and impressive degradation capability,especially with 77%refractory tetracycline and almost 100%rhodamine B degradedwithin an hour.The penetration ofCs+is demonstrated to be a mode of interlayer doping,and Cs–N bonds(especially with sp^(2) pyridine N in C═N–C),along with robust chemical interaction and electron exchange,are fabricated.This atomic configuration triggers the broadened spectral response,the improved charge migration,and the activated photocatalytic capacity.Furthermore,we evaluate the CCN/cadmium sulfide hybrid as a Z-scheme configuration,promoting the visible HER yield to 9.02 mmol g^(−1) h^(−1),which is the highest ever reported among all CCN systems.This work adds to the rapidly expanding field of manipulation strategies and supports further development of mediating served for photocatalysis.
基金the National Key Research and Development Program of China (2022YFB3803300)the open research fund of Songshan Lake Materials Laboratory (2021SLABFK02)the National Natural Science Foundation of China (21961160720)。
文摘Nowadays, the soar of photovoltaic performance of perovskite solar cells has set off a fever in the study of metal halide perovskite materials. The excellent optoelectronic properties and defect tolerance feature allow metal halide perovskite to be employed in a wide variety of applications. This article provides a holistic review over the current progress and future prospects of metal halide perovskite materials in representative promising applications, including traditional optoelectronic devices(solar cells, light-emitting diodes, photodetectors, lasers), and cutting-edge technologies in terms of neuromorphic devices(artificial synapses and memristors) and pressure-induced emission. This review highlights the fundamentals, the current progress and the remaining challenges for each application, aiming to provide a comprehensive overview of the development status and a navigation of future research for metal halide perovskite materials and devices.
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the National Key Research and Development Program of China(No.2018YFE0204000)the National Natural Science Foundation of China(Nos.U20A20206,51972300,62274155,and 21975245)+3 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB43000000)the Key Research Program of Frontier Science,Chinese Academy of Sciences(No.QYZDBSSWSLH006)K.L.appreciates the support from the Youth Innovation Promotion Association,the Chinese Academy of Sciences(No.2020114)the Beijing Nova Program(No.2020117).
文摘In organic solar cells,the singlet and triplet excitons dissociate into free charge carriers with different mechanisms due to their opposite spin state.Therefore,the ratio of the singlet and triplet excitons directly affects the photocurrent.Many methods were used to optimize the performance of the low-efficiency solar cell by improving the ratio of triplet excitons,which shows a long diffusion length.Here we observed that in high-efficiency systems,the proportion of singlet excitons under linearly polarized light excitation is higher than that of circularly polarized light.Since the singlet charge transfer state has lower binding energy than the triplet state,it makes a significant contribution to the charge carrier generation and enhancement of the photocurrent.Further,the positive magnetic field effect reflects that singlet excitons dissociation plays a major role in the photocurrent,which is opposite to the case of low-efficiency devices where triplet excitons dominate the photocurrent.
基金National Key Research and Development Program of China(2018YFE0204000)Strategic Priority Research Program of the Chinese Academy of Sciences(XDB43000000)+2 种基金National Natural Science Foundation of China(21975245,51972300,62274155,U20A20206)Youth Innovation Promotion Association of the Chinese Academy of Sciences(2020114)Beijing Nova Program(2020117)。
文摘Optical frequency combs(OFCs)have great potential in communications,especially in dense wavelength-division multiplexing.However,the size of traditional OFCs based on conventional optical microcavities or dispersion fibers is at least tens of micrometers,far larger than that of nanoscale electronic chips.Therefore,reducing the size of OFCs to match electronic chips is of necessity.Here,for the first time to our knowledge,we introduce surface plasmon polaritons(SPPs)to the construction of OFCs to realize a miniature device.The thickness of our device is reduced below 1μm.Though the presence of SPPs may induce ohmic and scattering loss,the threshold of the device is obtained as 9μW,comparable to the conventional device.Interestingly,the response time is 13.2 ps,much faster than the optical counterparts.This work provides a feasible strategy for the miniaturization of OFCs.
基金supported by the National Natural Science Foundation of China(No.41471410)the Key Beijing Discipline of Ecology(No.XK10019440)
文摘Earthworms have the ability to accumulate of heavy metals, however, there was few studies that addressed the metals in earthworm at subcellular levels in fields. The distributions of metals (Cd, Cu, Zn, and Pb) in subcellular fractions (cytosol, debris, and granules) of earthworm Metaphire californica were investigated. The relationship between soil metals and earthworms were analyzed to explain its high plasticity to inhabit in situ contaminated soil of Hunan Province, south China. The concentration of Cd in subcellular compartments showed the same pattern as Cu in the order of cytosol 〉 debris 〉 granules. The distribution of Zn and Pb in earthworms indicated a similar propensity for different subcellular fractions that ranked as granules 〉 debris 〉 cytosol for Zn, and granules 〉 cytosol 〉 debris for Pb. The internal metal concentrations in earthworms increased with the soil metals (p 〈 0.05). Significant positive correlations were found between soil Cd and Cd concentrations in cytosol and debris (p 〈 0.01). Moreover, the soil Pb concentration significantly influenced the Pb concentrations in cytosol and debris (p 〈 0.01), similar to that of Cd. The soil Cu concentrations was only associated with the Cu in granules (p 〈 0.05). Soil Zn concentrations correlated with the Zn concentrations in each subcellular fraction (p 〈 0.05). Our results provide insights into the variations of metals partitioning in earthworms at subcellular levels and the relationships of soil metals, which could be one of the detoxiflcation strategies to adapt the long-term contaminated environment.