Spatial separation of oxidation/reduction cocatalyst is an effective means to improve the efficiency of charge separation in photocatalytic reaction systems.Herein,a yolk-shell Pd@NH_(2)-UiO-66@Cu_(2)O heterojunction ...Spatial separation of oxidation/reduction cocatalyst is an effective means to improve the efficiency of charge separation in photocatalytic reaction systems.Herein,a yolk-shell Pd@NH_(2)-UiO-66@Cu_(2)O heterojunction was designed and synthesized by integration of electron collector Pd and hole collector Cu_(2)O inside and outside of a photoactive metal-organic framework(MOF)NH_(2)-UiO-66,respectively.The obtained Pd@NH_(2)-UiO-66@Cu_(2)O heterojunction effectively inhibits the electron and hole recombination through the photo-induced electrons and holes flow inward and outward of the composite,and promotes the reduction and oxidation abilities for the oxidative coupling of benzylamine to imines.Compared with Pd/NH_(2)-UiO-66@Cu_(2)O,Pd@NH_(2)-UiO-66,and Pd/NH_(2)-UiO-66,Pd@NH_(2)-UiO-66@Cu_(2)O exhibits the highest photocatalytic activity.More importantly,Pd@NH_(2)-UiO-66@Cu_(2)O shows a conversion rate of benzylamine up to 99%either by oxidation under aerobic conditions or by strong adsorption of H atom(Hads)under anaerobic conditions.In addition,the catalyst shows good stability and can be recycled at least ten times.This work provides useful guidance on construction of MOFs-based composites with spatially separated photoinduced charge carriers to realize efficient oxidation coupling of benzylamine in both aerobic and anaerobic conditions.展开更多
The oxygen evolution reaction(OER)with sluggish reaction kinetics and large overpotential is the critical reaction in water splitting that is promising for energy storage and conversion.Layered double hydroxides(LDHs)...The oxygen evolution reaction(OER)with sluggish reaction kinetics and large overpotential is the critical reaction in water splitting that is promising for energy storage and conversion.Layered double hydroxides(LDHs),due to their unique lamellar structure and flexibility of chemical component,are very competing material candidates for OER.Herein,the morphology structure and the electronic structure of LDHs were simultaneously tuned to improve the OER catalytic activity by mild solvothermal reduction using ethylene glycol.The increased surface area,the introduction of oxygen vacancies and the construction of hierarchical structure greatly enhanced the electro-catalytic activity of LDHs for OER.The as-prepared LDHs showed a lower over-potential as low as 276 mV at a current density of 10 mA cm-2,and a small Tafel slope of 40.3 mV dec-1 accompanied with good stability.This work provides an efficient way to the design and optimization of advanced catalysts in the future.展开更多
Electrochemical reactions were widely used in energy storage and conversion devices. The development of low-cost, highly efficient and stable electrocatalyst is essential to a large-scale application of energy storage...Electrochemical reactions were widely used in energy storage and conversion devices. The development of low-cost, highly efficient and stable electrocatalyst is essential to a large-scale application of energy storage and conversion devices. Recently, emerging plasma technology has been employed as one of the practical ways to synthesize and modify electrocatalysts due to its unique property. In this review, we summarized the latest applications of plasma in energy storage and conversion, including using it as the preparation and modification technology of the various electrocatalysts and the usage of it as the synthesis technology directly. Firstly, we presented the definition and types of plasma reactors and their respective characteristics. Then, these applications of plasma technology in many essential electrode reactions including carbon dioxide reduction reaction(CO_2RR), nitrogen fixation, oxygen reduction reaction(ORR), oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) were introduced.Finally, the challenges and outlook of plasma technology in energy storage and conversion were summarized, and the solutions and prospected its development in the future were present. Through reviewing the related aspects, readers can have a deeper understanding of the application prospects of plasma in electrocatalysis.展开更多
Emerging organic–inorganic metal halide perovskite materials have become the focus of the optoelectronics research community owing to their excellent photoelectric properties.Nevertheless,challenges still exist for t...Emerging organic–inorganic metal halide perovskite materials have become the focus of the optoelectronics research community owing to their excellent photoelectric properties.Nevertheless,challenges still exist for transferring the lab-made devices to largearea industrial modules.Inkjet printing(IJP)technology provides a promising way to fill the gap because of its precise droplet control and uniform large-scale deposition functions.Hence,an in-depth understanding of inkjet-printed perovskite films in terms of droplet manipulation and crystallization regulation is critical for upscaling the perovskite devices to commercial usage.In this review,we give an overview of inkjet-printed high-quality perovskite films and provide guidelines on inkjet-printing large-scale highperformance perovskite devices.First,we analyze theories of droplet formation and perovskite nucleation/crystallization dynamics and then focus on summarizing the perovskite film-formation strategies via IJP,in the aspects of ink engineering,the printing process,and posttreatment.Furthermore,we review the recent advances of inkjet-printed perovskite films on optoelectronic devices,such as perovskite solar cells,perovskite light-emitting diodes,and perovskite photodetectors.Finally,we highlight the“Trilogy Strategies,”including ink engineering,printing process,and posttreatment for printing high-quality perovskite films.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21771163 and 22171247)Zhongyuan thousand talents project.
文摘Spatial separation of oxidation/reduction cocatalyst is an effective means to improve the efficiency of charge separation in photocatalytic reaction systems.Herein,a yolk-shell Pd@NH_(2)-UiO-66@Cu_(2)O heterojunction was designed and synthesized by integration of electron collector Pd and hole collector Cu_(2)O inside and outside of a photoactive metal-organic framework(MOF)NH_(2)-UiO-66,respectively.The obtained Pd@NH_(2)-UiO-66@Cu_(2)O heterojunction effectively inhibits the electron and hole recombination through the photo-induced electrons and holes flow inward and outward of the composite,and promotes the reduction and oxidation abilities for the oxidative coupling of benzylamine to imines.Compared with Pd/NH_(2)-UiO-66@Cu_(2)O,Pd@NH_(2)-UiO-66,and Pd/NH_(2)-UiO-66,Pd@NH_(2)-UiO-66@Cu_(2)O exhibits the highest photocatalytic activity.More importantly,Pd@NH_(2)-UiO-66@Cu_(2)O shows a conversion rate of benzylamine up to 99%either by oxidation under aerobic conditions or by strong adsorption of H atom(Hads)under anaerobic conditions.In addition,the catalyst shows good stability and can be recycled at least ten times.This work provides useful guidance on construction of MOFs-based composites with spatially separated photoinduced charge carriers to realize efficient oxidation coupling of benzylamine in both aerobic and anaerobic conditions.
基金supported by the Fundamental Research Funds for the Central Universities (531107051102)the National Natural Science Foundation of China (51402100, 21573066, 21522305)+1 种基金the Provincial Natural Science Foundation of Hunan (2016TP1009)the Shenzhen Discovery Funding (JCYJ20170306141659388)
文摘The oxygen evolution reaction(OER)with sluggish reaction kinetics and large overpotential is the critical reaction in water splitting that is promising for energy storage and conversion.Layered double hydroxides(LDHs),due to their unique lamellar structure and flexibility of chemical component,are very competing material candidates for OER.Herein,the morphology structure and the electronic structure of LDHs were simultaneously tuned to improve the OER catalytic activity by mild solvothermal reduction using ethylene glycol.The increased surface area,the introduction of oxygen vacancies and the construction of hierarchical structure greatly enhanced the electro-catalytic activity of LDHs for OER.The as-prepared LDHs showed a lower over-potential as low as 276 mV at a current density of 10 mA cm-2,and a small Tafel slope of 40.3 mV dec-1 accompanied with good stability.This work provides an efficient way to the design and optimization of advanced catalysts in the future.
基金supported by the National Natural Science Foundation of China (Nos. 51402100 and 21573066)the Provincial Natural Science Foundation of Hunan (Nos. 2016JJ1006 and 2016TP1009)
文摘Electrochemical reactions were widely used in energy storage and conversion devices. The development of low-cost, highly efficient and stable electrocatalyst is essential to a large-scale application of energy storage and conversion devices. Recently, emerging plasma technology has been employed as one of the practical ways to synthesize and modify electrocatalysts due to its unique property. In this review, we summarized the latest applications of plasma in energy storage and conversion, including using it as the preparation and modification technology of the various electrocatalysts and the usage of it as the synthesis technology directly. Firstly, we presented the definition and types of plasma reactors and their respective characteristics. Then, these applications of plasma technology in many essential electrode reactions including carbon dioxide reduction reaction(CO_2RR), nitrogen fixation, oxygen reduction reaction(ORR), oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) were introduced.Finally, the challenges and outlook of plasma technology in energy storage and conversion were summarized, and the solutions and prospected its development in the future were present. Through reviewing the related aspects, readers can have a deeper understanding of the application prospects of plasma in electrocatalysis.
基金the financial support of the National Key R&D Program of China(grant no.2018YFA0208501)the National Natural Science Foundation of China(grant nos.51803217,51773206,91963212,2210090429,62104216,and 51961145102[BRICS project])+6 种基金Beijing National Laboratory for Molecular Sciences(grant nos.BNLMS-CXXM-202005 and 2019BMS20003)the K.C.Wong Education Foundationthe Beijing National Laboratory for Molecular Sciences(grant no.BNLMSCXXM-202005)the Key R&D and Promotion Project of Henan Province(grant no.192102210032)the Open Project of State Key Laboratory of Silicon Materials(grant no.SKL2019-10)the China Postdoctoral Innovative Talent Support Program(grant no.BX2021271)the Outstanding Young Talent Research Fund of Zhengzhou University.
文摘Emerging organic–inorganic metal halide perovskite materials have become the focus of the optoelectronics research community owing to their excellent photoelectric properties.Nevertheless,challenges still exist for transferring the lab-made devices to largearea industrial modules.Inkjet printing(IJP)technology provides a promising way to fill the gap because of its precise droplet control and uniform large-scale deposition functions.Hence,an in-depth understanding of inkjet-printed perovskite films in terms of droplet manipulation and crystallization regulation is critical for upscaling the perovskite devices to commercial usage.In this review,we give an overview of inkjet-printed high-quality perovskite films and provide guidelines on inkjet-printing large-scale highperformance perovskite devices.First,we analyze theories of droplet formation and perovskite nucleation/crystallization dynamics and then focus on summarizing the perovskite film-formation strategies via IJP,in the aspects of ink engineering,the printing process,and posttreatment.Furthermore,we review the recent advances of inkjet-printed perovskite films on optoelectronic devices,such as perovskite solar cells,perovskite light-emitting diodes,and perovskite photodetectors.Finally,we highlight the“Trilogy Strategies,”including ink engineering,printing process,and posttreatment for printing high-quality perovskite films.
