Electrocatalytic nitrate reduction reaction(NO_(3)RR)offers a unique rationale for green NH_(3) synthesis,yet the lack of high-efficiency NO_(3)RR catalysts remains a great challenge.In this work,we show that Au nanoc...Electrocatalytic nitrate reduction reaction(NO_(3)RR)offers a unique rationale for green NH_(3) synthesis,yet the lack of high-efficiency NO_(3)RR catalysts remains a great challenge.In this work,we show that Au nanoclusters anchored on TiO_(2) nanosheets can efficiently catalyze the conversion of NO_(3)RR-to-NH_(3) under ambient conditions,achieving a maximal Faradic efficiency of 91%,a peak yield rate of 1923μg·h^(-1)·mgcat.-1,and high durability over 10 consecutive cycles,all of which are comparable to the recently reported metrics(including transition metal and noble metal-based catalysts)and exceed those of pristine TiO_(2).Moreover,a galvanic Zn-nitrate battery using the catalyst as the cathode was proposed,which shows a power density of 3.62 mW·cm^(-2) and a yield rate of 452μg·h^(-1)·mgcat.-1.Theoretical simulations further indicate that the atomically dispersed Au clusters can promote the adsorption and activation of NO_(3)-species,and reduce the NO_(3)RR-to-NH_(3) barrier,thus leading to an accelerated cathodic reaction.This work highlights the importance of metal clusters for the NH_(3) electrosynthesis and nitrate removal.展开更多
Prussian blue(PB)is an anodic coloring candidate in the wide area of electrochromic(EC)applications.However,the co-influence of weak adhesion and low electrical conductivity leads to the poor stability and slow switch...Prussian blue(PB)is an anodic coloring candidate in the wide area of electrochromic(EC)applications.However,the co-influence of weak adhesion and low electrical conductivity leads to the poor stability and slow switching speed.To tackle this bottleneck,a novel TiO_(2)/Au/PB nanorod array is designed through hydrothermal and electrodeposition approaches on fluorine-doped tin oxide(FTO)glass.Such a designed ternary array structure could not only increase reactive site and conductivity,but also improve ion storage capacity and promote charge transfer,attributed to the synergistic effect of TiO_(2)/Au/PB core–shell heterostructure and the localized surface plasmon resonance(LSPR)effect of Au nanoparticles.Besides,density functional theory(DFT)calculation confirms the strong interaction between rutile TiO_(2)and FTO substrate,which contributes to the improvement of EC cycle stability.Benefiting from these effects,the TiO_(2)/Au/PB film shows a fast coloration/bleaching response of 1.08/2.01 s(2.17/4.48 s,PB film)and ultra-stable EC performance of 86.8%after 20,000 cycles(50%after 600 cycles,PB film).Furthermore,the high-intensity light source can be shot clearly by the designed and assembled EC iris device(ECID)with TiO_(2)/Au/PB film as an EC layer,while the photograph without an ECID is blurry,confirming the feasibility of the material in portable digital products.展开更多
The size of metal nanoparticles is a key factor to enhance the photocatalytic activity of photocatalysts.However,the mechanism of this factor to the improvement of photocatalytic CO_(2) reduction performance is still ...The size of metal nanoparticles is a key factor to enhance the photocatalytic activity of photocatalysts.However,the mechanism of this factor to the improvement of photocatalytic CO_(2) reduction performance is still unclear.Here,Au cluster/TiO_(2)/Ti_(3)C_(2) and Au nanoparticle/TiO_(2)/Ti_(3)C_(2) were successfully prepared by deposition-precipitation method.The experimental results show that the photocatalytic CO_(2) reduction performance of Au cluster/TiO_(2)/Ti_(3)C_(2) with quantum size effect is stronger than that of Au nanoparticle/TiO_(2)/Ti_(3)C_(2) with surface plasmon resonance.The enhanced photocatalytic CO_(2) reduction activity is assigned to the establishment of an overlapping orbital between the lowest unoccupied molecular orbital(LUMO)of the Au cluster and the anti-bonding orbital of CO_(2),which greatly promotes the activation efficiency of CO_(2).The existence of Au cluster and the mechanism of photocatalytic CO_(2) reduction performance were certified by high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)and in situ Fourier transform infrared spectroscopy(ISFTIR).This work may open new opportunities for the establishment of stable and active metal nanocatalysts.展开更多
TiO_(2)photocatalysts have been widely studied and applied for removing bacteria,but its antibacterial efficiency is limited to the ultraviolet(UV)range of the solar spectrum.In this work,we use the gold(Au)nanorods t...TiO_(2)photocatalysts have been widely studied and applied for removing bacteria,but its antibacterial efficiency is limited to the ultraviolet(UV)range of the solar spectrum.In this work,we use the gold(Au)nanorods to enhance the visible and near-infrared(NIR)light absorption of TiO_(2)NBs,a typical UV light photocatalyst,thus the enhancement of its full solar spectrum(UV,visible and NIR)photocatalytic antibacterial properties is achieved.Preliminary surface plasmon resonance(SPR)enhancement photocatalytic antibacterial mechanism is suggested.On one hand,transverse and longitudinal SPR of Au NRs is beneficial for visible and NIR light utilization.On the other hand,Au NRs combined with TiO_(2)NBs to form the heterostructure,which can improve the photogenerated carrier separation and direct electron transfer increases the hot electron concentration while Au NRs as the electron channel can well restrain charge recombination.finally produces the high yield of radical oxygen species and exhibits a superior antibacterial efficiency.Furthermore,we design a sterilization file cabinet with Au NR/TiO_(2)NB heterostructures as the photocatalytic coating plates.Our study reveals that Au NR/TiO_(2)NB heterostructure is a potential candidate for sterilization of bacteria and archives protection.展开更多
Au/TiO_(2) catalyst is firstly reported to be efficient in the hydrogenation of nitrobenzene to produce p-aminophenol with a high PAP selectivity of 81%and overall yield more than 63%.The catalyst is also quite stable...Au/TiO_(2) catalyst is firstly reported to be efficient in the hydrogenation of nitrobenzene to produce p-aminophenol with a high PAP selectivity of 81%and overall yield more than 63%.The catalyst is also quite stable and can be reused for at least 4 times with only slight decrease in activity.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22075211 and 51971157)the Guangzhou Basic&Applied Basic Research Project(No.202201011853)+2 种基金the Shenzhen Science and Technology Program(Nos.JCYJ20210324115412035,JCYJ20210324123202008,JCYJ20210324122803009,and ZDSYS20210813095534001)the Guangdong Basic and Applied Basic Research Foundation(No.2021A1515110880)the Tianjin Science Fund for Distinguished Young Scholars(No.19JCJQJC61800).
文摘Electrocatalytic nitrate reduction reaction(NO_(3)RR)offers a unique rationale for green NH_(3) synthesis,yet the lack of high-efficiency NO_(3)RR catalysts remains a great challenge.In this work,we show that Au nanoclusters anchored on TiO_(2) nanosheets can efficiently catalyze the conversion of NO_(3)RR-to-NH_(3) under ambient conditions,achieving a maximal Faradic efficiency of 91%,a peak yield rate of 1923μg·h^(-1)·mgcat.-1,and high durability over 10 consecutive cycles,all of which are comparable to the recently reported metrics(including transition metal and noble metal-based catalysts)and exceed those of pristine TiO_(2).Moreover,a galvanic Zn-nitrate battery using the catalyst as the cathode was proposed,which shows a power density of 3.62 mW·cm^(-2) and a yield rate of 452μg·h^(-1)·mgcat.-1.Theoretical simulations further indicate that the atomically dispersed Au clusters can promote the adsorption and activation of NO_(3)-species,and reduce the NO_(3)RR-to-NH_(3) barrier,thus leading to an accelerated cathodic reaction.This work highlights the importance of metal clusters for the NH_(3) electrosynthesis and nitrate removal.
基金Funds for the Central Universities(Nos.HIT.OCEF.2021004 and FRFCU5710090220).
文摘Prussian blue(PB)is an anodic coloring candidate in the wide area of electrochromic(EC)applications.However,the co-influence of weak adhesion and low electrical conductivity leads to the poor stability and slow switching speed.To tackle this bottleneck,a novel TiO_(2)/Au/PB nanorod array is designed through hydrothermal and electrodeposition approaches on fluorine-doped tin oxide(FTO)glass.Such a designed ternary array structure could not only increase reactive site and conductivity,but also improve ion storage capacity and promote charge transfer,attributed to the synergistic effect of TiO_(2)/Au/PB core–shell heterostructure and the localized surface plasmon resonance(LSPR)effect of Au nanoparticles.Besides,density functional theory(DFT)calculation confirms the strong interaction between rutile TiO_(2)and FTO substrate,which contributes to the improvement of EC cycle stability.Benefiting from these effects,the TiO_(2)/Au/PB film shows a fast coloration/bleaching response of 1.08/2.01 s(2.17/4.48 s,PB film)and ultra-stable EC performance of 86.8%after 20,000 cycles(50%after 600 cycles,PB film).Furthermore,the high-intensity light source can be shot clearly by the designed and assembled EC iris device(ECID)with TiO_(2)/Au/PB film as an EC layer,while the photograph without an ECID is blurry,confirming the feasibility of the material in portable digital products.
基金financially supported by the National Natural Science Foundation of China(Nos.51672099 and 52073263)Sichuan Science and Technology Program(No.2021JDTD0026)+1 种基金the Fundamental Research Funds for the Central Universities(No.2017-QR-25)the Research Team Project of Dongguan University of Technology(Nos.TDYB2019014 and TDQN2019011)。
文摘The size of metal nanoparticles is a key factor to enhance the photocatalytic activity of photocatalysts.However,the mechanism of this factor to the improvement of photocatalytic CO_(2) reduction performance is still unclear.Here,Au cluster/TiO_(2)/Ti_(3)C_(2) and Au nanoparticle/TiO_(2)/Ti_(3)C_(2) were successfully prepared by deposition-precipitation method.The experimental results show that the photocatalytic CO_(2) reduction performance of Au cluster/TiO_(2)/Ti_(3)C_(2) with quantum size effect is stronger than that of Au nanoparticle/TiO_(2)/Ti_(3)C_(2) with surface plasmon resonance.The enhanced photocatalytic CO_(2) reduction activity is assigned to the establishment of an overlapping orbital between the lowest unoccupied molecular orbital(LUMO)of the Au cluster and the anti-bonding orbital of CO_(2),which greatly promotes the activation efficiency of CO_(2).The existence of Au cluster and the mechanism of photocatalytic CO_(2) reduction performance were certified by high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)and in situ Fourier transform infrared spectroscopy(ISFTIR).This work may open new opportunities for the establishment of stable and active metal nanocatalysts.
基金fundings from the National Natural Science Foundation of China(Nos.51872173,51772176)TaishanScholars Program of Shandong Province(Nos.tsqn201812068,tspd20161006)+6 种基金Higher School Youth Innovation Team of Shandong Province(No.2019KJA013)Key Research and Development Program of Shandong Province(No.2018GGX102028)Science and Technology Special Project of Qingdao City(No.20-3-4-3-nsh)the Opening Fund of State Key Laboratory of Heavy Oil Processing(No.SKLOP202002006)Cooperative Education Project of the Ministry of Education(No.201902195026)Humanities and Social Sciences Program(GoMoruo Studies)of the Education Department of Sichuan Province(No.GY2020C01)Shandong Archives Science and Technology Project(No.2020-33)。
文摘TiO_(2)photocatalysts have been widely studied and applied for removing bacteria,but its antibacterial efficiency is limited to the ultraviolet(UV)range of the solar spectrum.In this work,we use the gold(Au)nanorods to enhance the visible and near-infrared(NIR)light absorption of TiO_(2)NBs,a typical UV light photocatalyst,thus the enhancement of its full solar spectrum(UV,visible and NIR)photocatalytic antibacterial properties is achieved.Preliminary surface plasmon resonance(SPR)enhancement photocatalytic antibacterial mechanism is suggested.On one hand,transverse and longitudinal SPR of Au NRs is beneficial for visible and NIR light utilization.On the other hand,Au NRs combined with TiO_(2)NBs to form the heterostructure,which can improve the photogenerated carrier separation and direct electron transfer increases the hot electron concentration while Au NRs as the electron channel can well restrain charge recombination.finally produces the high yield of radical oxygen species and exhibits a superior antibacterial efficiency.Furthermore,we design a sterilization file cabinet with Au NR/TiO_(2)NB heterostructures as the photocatalytic coating plates.Our study reveals that Au NR/TiO_(2)NB heterostructure is a potential candidate for sterilization of bacteria and archives protection.
基金Financial support by the Major State Basic Resource Development Program(Grant No.2012CB224804)NSFC(Project Nos.21373054,21173052)+1 种基金the Natural Science Foundation of Shanghai Science and Technol-ogy Committee(No.08DZ2270500)Hui-Chun Chin and Tsung-Dao Lee Chinese Undergraduate Re-search Endowment(CURE).
文摘Au/TiO_(2) catalyst is firstly reported to be efficient in the hydrogenation of nitrobenzene to produce p-aminophenol with a high PAP selectivity of 81%and overall yield more than 63%.The catalyst is also quite stable and can be reused for at least 4 times with only slight decrease in activity.
