The sluggish kinetics of the oxygen reduction reaction(ORR)and high over potential of oxygen evolution reaction(OER)are big challenges in the development of high-performance zinc-air batteries(ZABs)and fuel cells.In t...The sluggish kinetics of the oxygen reduction reaction(ORR)and high over potential of oxygen evolution reaction(OER)are big challenges in the development of high-performance zinc-air batteries(ZABs)and fuel cells.In this work,we report a rational design and a simple fabrication strategy of a photo-enhanced Co single-atom catalyst(SAC)comprising g-C3N4 coupled with cobalt-nitrogen-doped hierarchical mesoporous carbon(Co-N/MPC),forming a staggered p-n heterojunction that effectively improves charge separation and enhances electrocatalytic activity.The incorporation of Co SACs and g-C3N4 synergistically optimizes the photogenerated electron-hole pair separation,significantly boosting the intrinsic ORR-OER duplex activity.Under illumination,g-C_(3)N_(4)@Co-N/MPC exhibits an outstanding ORR half-wave potential(E1/2)of 0.841 V(vs.RHE)in 0.1 mol L^(–1)KOH and a low OER overpotential of 497.4 mV(vs.RHE)at 10 mA cm^(–2)in 1 mol L^(–1)KOH.Notably,the catalyst achieves an exceptional peak power density of 850.7 mW cm^(–2)in ZABs and of 411 mW cm^(–2)even in H_(2)-air fuel cell.In addition,g-C_(3)N_(4)@Co-N/MPC-based ZABs also show remarkable cycling stability exceeding 250 h.The advanced photo-induced charge separation at the p-n heterojunction facilitates faster electron transfer kinetics,and the mass transport owing to hierarchical mesoporous structure of Co-N-C,thereby reducing the overpotential and enhancing the overall energy conversion efficiency.This work provides a new perspective on designing next-generation of single-atom dispersed oxygen reaction catalysts,paving the way for high-performance photo-enhanced energy storage and conversion systems.展开更多
Zinc oxide(ZnO),as a broadband gap semiconductor material,exhibits unique physical and chemical properties that make it highly suitable for optoelectronics,piezoelectric devices,and gas-sensitive sensors,showing signi...Zinc oxide(ZnO),as a broadband gap semiconductor material,exhibits unique physical and chemical properties that make it highly suitable for optoelectronics,piezoelectric devices,and gas-sensitive sensors,showing significant potential for various applications.This paper focuses on the regulation and application of ZnO-based p-n junctions and piezoelectric devices.It discusses in detail the preparation of ZnO materials,the construction of p-n junctions,the optimization of piezoelectric device performance,and its application in various fields.By employing different preparation methods and strategies,high-quality ZnO thin films can be grown,and effective control of p-type conductivity achieved.This study provides both a theoretical foundation and technical support for controlling the performance of ZnO-based piezoelectric devices,as well as paving new pathways for the broader application of ZnO materials.展开更多
The p-n junction is the foundation building structure for manufacturing various electronic and optoelec-tronic devices.Ultrawide bandgap semiconductors are expected to overcome the limited power capability of Si-based...The p-n junction is the foundation building structure for manufacturing various electronic and optoelec-tronic devices.Ultrawide bandgap semiconductors are expected to overcome the limited power capability of Si-based electronic device,however,it is very difficult to achieve efficient bipolar doping due to the asymmetric doping effect,thereby impeding the development of p-n homojunction and related bipolar devices,especially for the Ga_(2)O_(3)-based materials and devices.Here,we demonstrate a unique one-step integrated growth of p-type N-doped(201)β-Ga_(2)O_(3)/n-type Si-doped(¯201)β-Ga_(2)O_(3)films by phase tran-sition and in-situ pre-doping of dopants,and fabrication of fullβ-Ga_(2)O_(3)linearly-graded p-n homojunc-tion diode from them.The fullβ-Ga_(2)O_(3)p-n homojunction diode possesses a large built-in potential of 4.52 eV,a high operation electric field>2.90 MV/cm in the reverse-bias regime,good longtime-stable rectifying behaviors with a rectification ratio of 104,and a high-speed switching and good surge robust-ness with a weak minority-carrier charge storage.Our work opens the way to the fabrication of Ga_(2)O_(3)-based p-n homojunction,lays the foundation for fullβ-Ga_(2)O_(3)-based bipolar devices,and paves the way for the novel fabrication of p-n homojunction for wide-bandgap oxides.展开更多
Despite advances in photocatalytic half-reduction reactions,challenges remain in effectively utilizing electron-hole pairs in concurrent redox processes.The present study involved the construction of a p-n junction Co...Despite advances in photocatalytic half-reduction reactions,challenges remain in effectively utilizing electron-hole pairs in concurrent redox processes.The present study involved the construction of a p-n junction Co_(3)O_(4)/Zn_(3)In_(2)S_(6)(CoZ)hybrid with a complementary band edge potential.The photocatalyst formed by the 2D assembled-nanostructure portrayed an optimal yield of 13.8(H_(2))and 13.1(benzaldehyde)mmol g^(-1)h^(-1)when exposed to light(λ>420 nm),surpassing 1%Pt-added ZIS(12.4(H_(2))and 10.71(benzaldehyde)mmol g^(-1)h^(-1)).Around 95%of the electron-hole utilization rate was achieved.The solar-to-hydrogen(STH)and apparent quantum yield(AQY)values of 0.466%and 4.96%(420nm)achieved by this system in the absence of sacrificial agents exceeded those of previous works.The exceptional performance was mostly ascribed to the synergistic development of adjoining p-n heterojunctions and the built-in electric field for effective charge separation.Moreover,scavenger studies elucidated the intricate mechanistic enigma of the dual-redox process,in which benzaldehyde was produced via O-H activation and subsequent C-H cleavage of benzyl alcohol over CoZ hybrids.Furthermore,the widespread use of the optimal 1-CoZ composites was confirmed in multiple photoredox systems.This work presents an innovative perspective on the construction of dual-functioning p-n heterojunctions for practical photoredox applications.展开更多
Photosensors with versatile functionalities have emerged as a cornerstone for breakthroughs in the future optoelectronic systems across a wide range of applications.In particular,emerging photoelectrochemical(PEC)-typ...Photosensors with versatile functionalities have emerged as a cornerstone for breakthroughs in the future optoelectronic systems across a wide range of applications.In particular,emerging photoelectrochemical(PEC)-type devices have recently attracted extensive interest in liquid-based biosensing applications due to their natural electrolyte-assisted operating characteristics.Herein,a PEC-type photosensor was carefully designed and constructed by employing gallium nitride(GaN)p-n homojunction semiconductor nanowires on silicon,with the p-GaN segment strategically doped and then decorated with cobalt-nickel oxide(CoNiO_(x)).Essentially,the p-n homojunction configuration with facile p-doping engineering improves carrier separation efficiency and facilitates carrier transfer to the nanowire surface,while CoNiO_(x)decoration further boosts PEC reaction activity and carrier dynamics at the nanowire/electrolyte interface.Consequently,the constructed photosensor achieves a high responsivity of 247.8 mA W^(-1)while simultaneously exhibiting excellent operating stability.Strikingly,based on the remarkable stability and high responsivity of the device,a glucose sensing system was established with a demonstration of glucose level determination in real human serum.This work offers a feasible and universal approach in the pursuit of high-performance bio-related sensing applications via a rational design of PEC devices in the form of nanostructured architecture with strategic doping engineering.展开更多
Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport...Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport and thus recombination loss at buried interface.Herein,we demonstrate an effective strategy of laser embedding of p-n homojunctions in the TiO_(2)ETL to accelerate electron transport in PSCs,through localized build-in electric fields that enables boosted electron mobility by two orders of magnitude.Such embedding is found significantly helpful for not only the enhanced crystallization quality of TiO_(2)ETL,but the fabrication of perovskite films with larger-grain and the less-trap-states.The embedded p-n homojunction enables also the modulation of interfacial energy level between perovskite layers and ETLs,favoring for the reduced voltage deficit of PSCs.Benefiting from these merits,the formamidinium lead iodide(FAPbI_(3))PSCs employing such ETLs deliver a champion efficiency of 25.50%,along with much-improved device stability under harsh conditions,i.e.,maintain over 95%of their initial efficiency after operation at maximum power point under continuous heat and illumination for 500 h,as well as mixed-cation PSCs with a champion efficiency of 22.02%and over 3000 h of ambient storage under humidity stability of 40%.Present study offers new possibilities of regulating charge transport layers via p-n homojunction embedding for high performance optoelectronics.展开更多
Carbon nitride(CN)-based heterojunction photocatalysts hold promise for efficient carbon dioxide(CO_(2))reduction.However,suboptimal production yields and limited selectivity in CO_(2)conversion pose significant barri...Carbon nitride(CN)-based heterojunction photocatalysts hold promise for efficient carbon dioxide(CO_(2))reduction.However,suboptimal production yields and limited selectivity in CO_(2)conversion pose significant barriers to achieving efficient CO_(2)conversion.Here,we present the construction of a p-n heterojunction between ultrasmall Te NPs and CN nanosheet using a novel tandem hydrothermal-calcination synthesis strategy.Through ammonia-assisted calcination,ultrasmall Te NPs are grown in-situ on the CN nanosheets’surface,resulting in the generation of a robust p-n heterojunction.The synthesized heterojunction exhibits increased specific surface area,reinforced visible light absorption,intensive CO_(2)adsorption capacity,and efficient charge transfer.The optimum Te/CN-NH_(3)demonstrates superior photocatalytic CO_(2)reduction activity and durability,with nearly 100%selectivity for CO and a yield as high as 92.0μmol g^(-1)h^(-1),a fourfold increase compared to pure CN.Experimental and theoretical calculations unravel that the strong built-in electric field of the Te/CN-NH_(3)p-n heterojunction accelerates the migration of photogenerated electrons from Te NPs to the N site on CN nanosheets,thereby promoting CO_(2)reduction.This study provides a promising material design approach for the construction of highperformance p-n heterojunction photocatalysts.展开更多
文摘The sluggish kinetics of the oxygen reduction reaction(ORR)and high over potential of oxygen evolution reaction(OER)are big challenges in the development of high-performance zinc-air batteries(ZABs)and fuel cells.In this work,we report a rational design and a simple fabrication strategy of a photo-enhanced Co single-atom catalyst(SAC)comprising g-C3N4 coupled with cobalt-nitrogen-doped hierarchical mesoporous carbon(Co-N/MPC),forming a staggered p-n heterojunction that effectively improves charge separation and enhances electrocatalytic activity.The incorporation of Co SACs and g-C3N4 synergistically optimizes the photogenerated electron-hole pair separation,significantly boosting the intrinsic ORR-OER duplex activity.Under illumination,g-C_(3)N_(4)@Co-N/MPC exhibits an outstanding ORR half-wave potential(E1/2)of 0.841 V(vs.RHE)in 0.1 mol L^(–1)KOH and a low OER overpotential of 497.4 mV(vs.RHE)at 10 mA cm^(–2)in 1 mol L^(–1)KOH.Notably,the catalyst achieves an exceptional peak power density of 850.7 mW cm^(–2)in ZABs and of 411 mW cm^(–2)even in H_(2)-air fuel cell.In addition,g-C_(3)N_(4)@Co-N/MPC-based ZABs also show remarkable cycling stability exceeding 250 h.The advanced photo-induced charge separation at the p-n heterojunction facilitates faster electron transfer kinetics,and the mass transport owing to hierarchical mesoporous structure of Co-N-C,thereby reducing the overpotential and enhancing the overall energy conversion efficiency.This work provides a new perspective on designing next-generation of single-atom dispersed oxygen reaction catalysts,paving the way for high-performance photo-enhanced energy storage and conversion systems.
基金The Natural Science Foundation of Guangdong Province(Project No.2023A1515012352)。
文摘Zinc oxide(ZnO),as a broadband gap semiconductor material,exhibits unique physical and chemical properties that make it highly suitable for optoelectronics,piezoelectric devices,and gas-sensitive sensors,showing significant potential for various applications.This paper focuses on the regulation and application of ZnO-based p-n junctions and piezoelectric devices.It discusses in detail the preparation of ZnO materials,the construction of p-n junctions,the optimization of piezoelectric device performance,and its application in various fields.By employing different preparation methods and strategies,high-quality ZnO thin films can be grown,and effective control of p-type conductivity achieved.This study provides both a theoretical foundation and technical support for controlling the performance of ZnO-based piezoelectric devices,as well as paving new pathways for the broader application of ZnO materials.
基金supported by the National Key R&D Program of China(Grant Nos.2022YFB3605500 and 2022YFB3605503).
文摘The p-n junction is the foundation building structure for manufacturing various electronic and optoelec-tronic devices.Ultrawide bandgap semiconductors are expected to overcome the limited power capability of Si-based electronic device,however,it is very difficult to achieve efficient bipolar doping due to the asymmetric doping effect,thereby impeding the development of p-n homojunction and related bipolar devices,especially for the Ga_(2)O_(3)-based materials and devices.Here,we demonstrate a unique one-step integrated growth of p-type N-doped(201)β-Ga_(2)O_(3)/n-type Si-doped(¯201)β-Ga_(2)O_(3)films by phase tran-sition and in-situ pre-doping of dopants,and fabrication of fullβ-Ga_(2)O_(3)linearly-graded p-n homojunc-tion diode from them.The fullβ-Ga_(2)O_(3)p-n homojunction diode possesses a large built-in potential of 4.52 eV,a high operation electric field>2.90 MV/cm in the reverse-bias regime,good longtime-stable rectifying behaviors with a rectification ratio of 104,and a high-speed switching and good surge robust-ness with a weak minority-carrier charge storage.Our work opens the way to the fabrication of Ga_(2)O_(3)-based p-n homojunction,lays the foundation for fullβ-Ga_(2)O_(3)-based bipolar devices,and paves the way for the novel fabrication of p-n homojunction for wide-bandgap oxides.
基金support provided by the Ministry of Higher Education Malaysia under the Fundamental Research Grant Scheme(FRGS)(No.FRGS/1/2024/TK08/XMU/02/1)supported by the PETRONAS-Academia Collaboration Dialogue(PACD 2023)grant,provided by PETRONAS Research Sdn.Bhd.(PRSB)+6 种基金the Ministry of Science,Technology and Innovation(MOSTI)Malaysia under the Strategic Research Fund(SRF)(S.22015)supported by the National Natural Science Foundation of China(No.22202168)Guangdong Basic and Applied Basic Research Foundation(No.2021A1515111019)support from the State Key Laboratory of Physical Chemistry of Solid Surfaces,Xiamen University(No.2023X11)supported by the Embassy of the People's Republic of China in Malaysia(EENG/0045)funded by Xiamen University Malaysia Investigatorship Grant(No.IENG/0038)Xiamen University Malaysia Research Fund(ICOE/0001,XMUMRF/2021-C8/IENG/0041 and XMUMRF/2025-C15/IENG/0080).
文摘Despite advances in photocatalytic half-reduction reactions,challenges remain in effectively utilizing electron-hole pairs in concurrent redox processes.The present study involved the construction of a p-n junction Co_(3)O_(4)/Zn_(3)In_(2)S_(6)(CoZ)hybrid with a complementary band edge potential.The photocatalyst formed by the 2D assembled-nanostructure portrayed an optimal yield of 13.8(H_(2))and 13.1(benzaldehyde)mmol g^(-1)h^(-1)when exposed to light(λ>420 nm),surpassing 1%Pt-added ZIS(12.4(H_(2))and 10.71(benzaldehyde)mmol g^(-1)h^(-1)).Around 95%of the electron-hole utilization rate was achieved.The solar-to-hydrogen(STH)and apparent quantum yield(AQY)values of 0.466%and 4.96%(420nm)achieved by this system in the absence of sacrificial agents exceeded those of previous works.The exceptional performance was mostly ascribed to the synergistic development of adjoining p-n heterojunctions and the built-in electric field for effective charge separation.Moreover,scavenger studies elucidated the intricate mechanistic enigma of the dual-redox process,in which benzaldehyde was produced via O-H activation and subsequent C-H cleavage of benzyl alcohol over CoZ hybrids.Furthermore,the widespread use of the optimal 1-CoZ composites was confirmed in multiple photoredox systems.This work presents an innovative perspective on the construction of dual-functioning p-n heterojunctions for practical photoredox applications.
基金funded by the National Natural Science Foundation of China(Grant Nos.62322410,52272168,52161145404,81974530,and 82271721)the Fundamental Research Funds for the Central Universities(Grant No.WK3500000009)+1 种基金the International Projects of the Chinese Academy of Science(CAS)under Grant No.211134KYSB20210011Hubei Provincial Science and Technology Innovation Talents and Services Special Program(Grant No.2022EHB039)。
文摘Photosensors with versatile functionalities have emerged as a cornerstone for breakthroughs in the future optoelectronic systems across a wide range of applications.In particular,emerging photoelectrochemical(PEC)-type devices have recently attracted extensive interest in liquid-based biosensing applications due to their natural electrolyte-assisted operating characteristics.Herein,a PEC-type photosensor was carefully designed and constructed by employing gallium nitride(GaN)p-n homojunction semiconductor nanowires on silicon,with the p-GaN segment strategically doped and then decorated with cobalt-nickel oxide(CoNiO_(x)).Essentially,the p-n homojunction configuration with facile p-doping engineering improves carrier separation efficiency and facilitates carrier transfer to the nanowire surface,while CoNiO_(x)decoration further boosts PEC reaction activity and carrier dynamics at the nanowire/electrolyte interface.Consequently,the constructed photosensor achieves a high responsivity of 247.8 mA W^(-1)while simultaneously exhibiting excellent operating stability.Strikingly,based on the remarkable stability and high responsivity of the device,a glucose sensing system was established with a demonstration of glucose level determination in real human serum.This work offers a feasible and universal approach in the pursuit of high-performance bio-related sensing applications via a rational design of PEC devices in the form of nanostructured architecture with strategic doping engineering.
基金financially supported by the project of the National Natural Science Foundation of China(52202115 and 52172101)the China Postdoctoral Science Foundation(2022M722586)+2 种基金the Natural Science Foundation of Chongqing,China(CSTB2022NSCQ-MSX1085)the Shaanxi Science and Technology Innovation Team(2023-CX-TD-44)the Fundamental Research Funds for the Central Universities(3102019JC005 and G2022KY0604)。
文摘Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport and thus recombination loss at buried interface.Herein,we demonstrate an effective strategy of laser embedding of p-n homojunctions in the TiO_(2)ETL to accelerate electron transport in PSCs,through localized build-in electric fields that enables boosted electron mobility by two orders of magnitude.Such embedding is found significantly helpful for not only the enhanced crystallization quality of TiO_(2)ETL,but the fabrication of perovskite films with larger-grain and the less-trap-states.The embedded p-n homojunction enables also the modulation of interfacial energy level between perovskite layers and ETLs,favoring for the reduced voltage deficit of PSCs.Benefiting from these merits,the formamidinium lead iodide(FAPbI_(3))PSCs employing such ETLs deliver a champion efficiency of 25.50%,along with much-improved device stability under harsh conditions,i.e.,maintain over 95%of their initial efficiency after operation at maximum power point under continuous heat and illumination for 500 h,as well as mixed-cation PSCs with a champion efficiency of 22.02%and over 3000 h of ambient storage under humidity stability of 40%.Present study offers new possibilities of regulating charge transport layers via p-n homojunction embedding for high performance optoelectronics.
基金funded by China Postdoctoral Science Foundation(2023T160406)Shanghai Pujiang Program(21PJD022)+1 种基金This project was also supported by Singapore Ministry of Education AcRF Tier 2(MOE-MOET2EP10121-0006)and AcRF Tier 1(RG7/21)This work is Supported by Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University.
文摘Carbon nitride(CN)-based heterojunction photocatalysts hold promise for efficient carbon dioxide(CO_(2))reduction.However,suboptimal production yields and limited selectivity in CO_(2)conversion pose significant barriers to achieving efficient CO_(2)conversion.Here,we present the construction of a p-n heterojunction between ultrasmall Te NPs and CN nanosheet using a novel tandem hydrothermal-calcination synthesis strategy.Through ammonia-assisted calcination,ultrasmall Te NPs are grown in-situ on the CN nanosheets’surface,resulting in the generation of a robust p-n heterojunction.The synthesized heterojunction exhibits increased specific surface area,reinforced visible light absorption,intensive CO_(2)adsorption capacity,and efficient charge transfer.The optimum Te/CN-NH_(3)demonstrates superior photocatalytic CO_(2)reduction activity and durability,with nearly 100%selectivity for CO and a yield as high as 92.0μmol g^(-1)h^(-1),a fourfold increase compared to pure CN.Experimental and theoretical calculations unravel that the strong built-in electric field of the Te/CN-NH_(3)p-n heterojunction accelerates the migration of photogenerated electrons from Te NPs to the N site on CN nanosheets,thereby promoting CO_(2)reduction.This study provides a promising material design approach for the construction of highperformance p-n heterojunction photocatalysts.
