Photoelectrochemical(PEC)water splitting is considered as an ideal technology to produce hydrogen.Photogenerated carrier migration is one of the most important roles in the whole process of PEC water splitting.It incl...Photoelectrochemical(PEC)water splitting is considered as an ideal technology to produce hydrogen.Photogenerated carrier migration is one of the most important roles in the whole process of PEC water splitting.It includes bulk transfer inside of the photoelectrode and the exchange at the solid-liquid interface.The energy barriers during the migration process lead to the dramatic recombination of photogenerated hot carrier and the reducing of their redox capacity.Thus,an applied bias voltage should be provided to overcome these energy barriers,which brings the additional loss of energy.Plentiful researches indicate that some methods for the regulation of photogenerated hot carrier,such as p-n junction,unique transfer nanochannel,tandem nanostructure and Z-Scheme transfer structure et al.,show great potential to achieve high-efficient PEC water overall splitting without any applied bias voltage.Up to now,many reviews have summarized and analyzed the methods to enhance the PEC or photocatalysis water splitting from the perspectives of materials,nanostructures and surface modification etc.However,few of them focus on the topic of photogenerated carrier transfer regulation,which is an important and urgent developing technique.For this reason,this review focuses on the regulation of photogenerated carriers generated by the photoelectrodes and summarizes different advanced methods for photogenerated carrier regulation developed in recent years.Some comments and outlooks are also provided at the end of this review.展开更多
Photogenerated charge separation and transfer is one of the bottleneck steps in photocatalysis,and efficient charge separation strategies are strongly desired.Here,mimicking the electron transport chain in natural pho...Photogenerated charge separation and transfer is one of the bottleneck steps in photocatalysis,and efficient charge separation strategies are strongly desired.Here,mimicking the electron transport chain in natural photosynthesis,we report the design and fabrication of a charge transfer chain using bismuth-based semiconductor as a proof-of-concept.In view of the thermodynamic energy band positions and structural similarity based on the density functional theory(DFT)analysis,heterostructured combination ofα-Bi_(2)O_(3),perovskite-like Bi_(4)Ti_(3)O_(12),and sillenite Bi12TiO20 was designed for fabrication of charge transfer chain.By tuning the molar ratio of Bi and Ti precursors,the Bi_(4)Ti_(3)O_(12)and Bi12TiO20 particles were formed on the surface ofα-Bi_(2)O_(3)by an insitu transformation process,giving rise to Bi_(12)TiO_(20)-Bi_(4)Ti_(3)O_(12)/α-Bi_(2)O_(3)composites with charge transfer chain.We propose that the effective charge transfer is accomplished amongα-Bi_(2)O_(3),Bi12TiO20,and Bi_(4)Ti_(3)O_(12),which significantly improves the photogenerated charge separation and transfer,as indicated by photoluminescene,time-resolved photoluminescene,and electrochemical impedance spectra results.As expected,the Bi_(12)TiO_(20)-Bi_(4)Ti_(3)O_(12)/α-Bi_(2)O_(3)shows the superior photocatalytic activity for the degradation of environmental pollutants with high concentration.Even for the refractory pollutants like 4-chlorophenol,the optimal Bi_(12)TiO_(20)-Bi_(4)Ti_(3)O_(12)/α-Bi_(2)O_(3)composite shows 28 times higher than that ofα-Bi_(2)O_(3)for photocatalytic degradation,verifying the superiority of photogenerated charge transfer chain in photocatalysis.This work demonstrates the feasibility of the charge transfer chain strategy to boost the photogenerated charge separation,which is of great significance for designing energy and environmental-related materials in heterogonous photocatalysis.展开更多
H_(2)O_(2)has been widely applied in the fields of chemical synthesis,medical sterilization,pollutant removal,etc.,due to its strong oxidizing property and the avoidable secondary pollution.Despite of the enhanced per...H_(2)O_(2)has been widely applied in the fields of chemical synthesis,medical sterilization,pollutant removal,etc.,due to its strong oxidizing property and the avoidable secondary pollution.Despite of the enhanced performance for H_(2)O_(2)generation over g-C_(3)N_(4)semiconductors through promoting the separation of photo-generated charge carriers,the effect of migration orientation of charge carriers is still ambiguous.For this emotion,surface modification of g-C_(3)N_(4)was employed to adjust the migration orientation of charge carriers,in order to investigate systematically its effect on the performance of H_(2)O_(2)generation.It was found that ultrathin g-C_(3)N_(4)(UCN)modified by boron nitride(BN),as an effective hole-attract agent,demonstrated a significantly enhanced performance.Particularly,for the optimum UCN/BN-40%catalyst,4.0-fold higher yield of H_(2)O_(2)was obtained in comparison with the pristine UCN.As comparison,UCN modified by carbon dust demonstrated a completely opposite tendency.The remarkably improved performance over UCN/BN was ascribed to the fact that more photo-generated electrons were remained inside of triazine structure of g-C_(3)N_(4),leading to the formation of larger amount of 1,4-endoxide.It is anticipated that our work could provide new insights for the design of photocatalyst with significantly improved performance for H_(2)O_(2)generation.展开更多
A series of Eu3+ -incorporated ETS-10 samples were successfully prepared based on the traditional ion exchange method. The relationship between photogenerated charge behaviors and luminescent properties has been inves...A series of Eu3+ -incorporated ETS-10 samples were successfully prepared based on the traditional ion exchange method. The relationship between photogenerated charge behaviors and luminescent properties has been investigated in detail. It has been demonstrated that as a result of the charge transfer from the titanate quantum wires to Eu3+ crystal field states, the host matrix ETS-10 functions as the sensitizer of Eu3+ to enhance the red luminescence, while Eu3+ cations contribute to the recombination of photogenerated charges. The behavior of photogenerated charges has significant impact on the luminescent properties of Eu3+ -incorporated ETS-10 materials.展开更多
基金financially supported by the National Natural Science Foundation of China,China(Grant Nos.41506093)。
文摘Photoelectrochemical(PEC)water splitting is considered as an ideal technology to produce hydrogen.Photogenerated carrier migration is one of the most important roles in the whole process of PEC water splitting.It includes bulk transfer inside of the photoelectrode and the exchange at the solid-liquid interface.The energy barriers during the migration process lead to the dramatic recombination of photogenerated hot carrier and the reducing of their redox capacity.Thus,an applied bias voltage should be provided to overcome these energy barriers,which brings the additional loss of energy.Plentiful researches indicate that some methods for the regulation of photogenerated hot carrier,such as p-n junction,unique transfer nanochannel,tandem nanostructure and Z-Scheme transfer structure et al.,show great potential to achieve high-efficient PEC water overall splitting without any applied bias voltage.Up to now,many reviews have summarized and analyzed the methods to enhance the PEC or photocatalysis water splitting from the perspectives of materials,nanostructures and surface modification etc.However,few of them focus on the topic of photogenerated carrier transfer regulation,which is an important and urgent developing technique.For this reason,this review focuses on the regulation of photogenerated carriers generated by the photoelectrodes and summarizes different advanced methods for photogenerated carrier regulation developed in recent years.Some comments and outlooks are also provided at the end of this review.
基金supported by the National Natural Science Foundation of China(No.22172068)the Natural Science Foundation of Jiangsu Province(No.BK20221485)+2 种基金the Liaoning Revitalization Talents Program(No.XLYC1902065)the Scientific Research Fund of Liaoning Provincial Department of Education(No.LJKMZ20220747)the Talent Scientific Research Fund of LSHU(No.2016XJJ-012).
文摘Photogenerated charge separation and transfer is one of the bottleneck steps in photocatalysis,and efficient charge separation strategies are strongly desired.Here,mimicking the electron transport chain in natural photosynthesis,we report the design and fabrication of a charge transfer chain using bismuth-based semiconductor as a proof-of-concept.In view of the thermodynamic energy band positions and structural similarity based on the density functional theory(DFT)analysis,heterostructured combination ofα-Bi_(2)O_(3),perovskite-like Bi_(4)Ti_(3)O_(12),and sillenite Bi12TiO20 was designed for fabrication of charge transfer chain.By tuning the molar ratio of Bi and Ti precursors,the Bi_(4)Ti_(3)O_(12)and Bi12TiO20 particles were formed on the surface ofα-Bi_(2)O_(3)by an insitu transformation process,giving rise to Bi_(12)TiO_(20)-Bi_(4)Ti_(3)O_(12)/α-Bi_(2)O_(3)composites with charge transfer chain.We propose that the effective charge transfer is accomplished amongα-Bi_(2)O_(3),Bi12TiO20,and Bi_(4)Ti_(3)O_(12),which significantly improves the photogenerated charge separation and transfer,as indicated by photoluminescene,time-resolved photoluminescene,and electrochemical impedance spectra results.As expected,the Bi_(12)TiO_(20)-Bi_(4)Ti_(3)O_(12)/α-Bi_(2)O_(3)shows the superior photocatalytic activity for the degradation of environmental pollutants with high concentration.Even for the refractory pollutants like 4-chlorophenol,the optimal Bi_(12)TiO_(20)-Bi_(4)Ti_(3)O_(12)/α-Bi_(2)O_(3)composite shows 28 times higher than that ofα-Bi_(2)O_(3)for photocatalytic degradation,verifying the superiority of photogenerated charge transfer chain in photocatalysis.This work demonstrates the feasibility of the charge transfer chain strategy to boost the photogenerated charge separation,which is of great significance for designing energy and environmental-related materials in heterogonous photocatalysis.
基金supported by the National Natural Science Foundation of China(No.21906132)Department of Science and Technology of Sichuan Province(Nos.2020YFG0158 and 2020YFH0162)the Engineering Research Center for the Development of Farmland Ecosystem Service Functions,Sichuan Province Institutions of Higher Education.
文摘H_(2)O_(2)has been widely applied in the fields of chemical synthesis,medical sterilization,pollutant removal,etc.,due to its strong oxidizing property and the avoidable secondary pollution.Despite of the enhanced performance for H_(2)O_(2)generation over g-C_(3)N_(4)semiconductors through promoting the separation of photo-generated charge carriers,the effect of migration orientation of charge carriers is still ambiguous.For this emotion,surface modification of g-C_(3)N_(4)was employed to adjust the migration orientation of charge carriers,in order to investigate systematically its effect on the performance of H_(2)O_(2)generation.It was found that ultrathin g-C_(3)N_(4)(UCN)modified by boron nitride(BN),as an effective hole-attract agent,demonstrated a significantly enhanced performance.Particularly,for the optimum UCN/BN-40%catalyst,4.0-fold higher yield of H_(2)O_(2)was obtained in comparison with the pristine UCN.As comparison,UCN modified by carbon dust demonstrated a completely opposite tendency.The remarkably improved performance over UCN/BN was ascribed to the fact that more photo-generated electrons were remained inside of triazine structure of g-C_(3)N_(4),leading to the formation of larger amount of 1,4-endoxide.It is anticipated that our work could provide new insights for the design of photocatalyst with significantly improved performance for H_(2)O_(2)generation.
基金supported by the National Natural Science Foundation of China (21201121, 21271128)the National Basic Research Program of China (2011CB808703)
文摘A series of Eu3+ -incorporated ETS-10 samples were successfully prepared based on the traditional ion exchange method. The relationship between photogenerated charge behaviors and luminescent properties has been investigated in detail. It has been demonstrated that as a result of the charge transfer from the titanate quantum wires to Eu3+ crystal field states, the host matrix ETS-10 functions as the sensitizer of Eu3+ to enhance the red luminescence, while Eu3+ cations contribute to the recombination of photogenerated charges. The behavior of photogenerated charges has significant impact on the luminescent properties of Eu3+ -incorporated ETS-10 materials.
基金supported by the National Natural Science Foundation of China(20837001 and 21077018)the Program for Changjiang Scholars and Innovative Research Team in University(IRT0813)~~
