CuInS2 semiconductor nanocrystals (NCs) exhibit large absorption coefficient, size-dependent photoluminescence and low toxicity, making them excellent candidates in a variety of bioapplications. However, precise contr...CuInS2 semiconductor nanocrystals (NCs) exhibit large absorption coefficient, size-dependent photoluminescence and low toxicity, making them excellent candidates in a variety of bioapplications. However, precise control of both their composition and morphology to improve the luminescent efficiency remains a great challenge via conventional direct synthesis. Herein, we present a novel low-temperature template synthesis of highly efficient luminescent CuInS2 nanoprobes from In2S3 NCs via a facile cation exchange strategy. The proposed strategy enables synthesis of a series of CuInS2 NCs with broad size tunability from 2.2 to 29.6 nm. Through rationally manipulating the stoichiometry of Cu/In, highly efficient luminescence of CuInS2 with the maximum quantum yield of 28.6% has been achieved, which is about one order of magnitude improvement relative to that of directly synthesized NCs. By virtue of the intense emission of CuInS2 nanoprobes, we exemplify their application in sensitive homogeneous biodetection for an important biomolecule of adenosine triphosphate (ATP) with the limit of detection down to 49.3 nM. Moreover, the CuInS2 nanoprobes are explored for ATP-targeted cancer cell imaging, thus revealing their great potentials in the field of cancer diagnosis and prognosis.展开更多
Crystal phase engineering on CulnS2(CIS)nanocrystals,especially polytypic structure,has become one of the research hotspots to design the advanced materials and devices for energy conversion and environment treatment....Crystal phase engineering on CulnS2(CIS)nanocrystals,especially polytypic structure,has become one of the research hotspots to design the advanced materials and devices for energy conversion and environment treatment.Here,the polytypic CIS nanosheets(NSs)including zincblende/wutzite and chalcopyrite/wurtzite types were first time achieved in a hot-injection system using oleic acid and liquid paraffin as the reaction media.As-obtained polytypic CIS NSs exhibit significantly enhanced light-absorption abillty and visible-light-driven photocatalytic performance originating from the rational hetero-crystalline interfaces and surface defect states,which efficiently inhibit the recombination of photo-generated carriers.Meanwhile,the polytypic CIS NSs were spin-coated onto the surface of fluorinated-tin oxide glass substrate and used as the photoelectrode,which shows an excellent photoelectrochemical(PEC)activity in aqueous solution.The present work not only provides a facile,rapid,low-cost,and environmental-friendly synthesis strategy to design the crystal phase and defect structure of ternary chalcogenides,but also demonstrates the relationships between the polytypic structure and photocatalytic/photoelectrochemical properties.展开更多
The sharp rise of CO2 in the atmosphere has become a potential threat to global climate, which results from the massive utilization of fossil fuel since the industry revolution. CO2 electroreduction provides us a new ...The sharp rise of CO2 in the atmosphere has become a potential threat to global climate, which results from the massive utilization of fossil fuel since the industry revolution. CO2 electroreduction provides us a new possibility of utilizing CO2 as a carbon feedstock for fuel and commercial chemicals generation. In this article, a new method is developed for synthesizing CuInS2 hollow nanostructures through the Kirkendall effect. The CuInS2 hollow nanostructures exhibit excellent catalytic activity for electrochemical reduction of CO2 with particular high selectivity, achieving high faradaic efficiency for HCOOH of 72.8% at -0.7 V. To elucidate the mechanisms, operando electrochemical Raman spectroscopy is employed to examine the CO2 reduction process. This work provides new insights into the design of hollow nanostructures toward electrocatalytic CO2 conversion and offers us an effective and reliable way for real-time investigation of electrochemical CO2 reduction reaction processes.展开更多
基金Foundation items:National Nature Science Foundation of China(50972107,51172165)Zhejinag Province Key Scientific and Technological Innovations Team of China(2009R50010)+1 种基金Key Foundation of Zhejiang Province Natural Science Foundation of China(Z4110347)Wenzhou Municipal Science and Technology Bureau Key Program(G20090082)
基金National Nature Science Foundation of China(50972107,51272059)Zhejinag Province Key Scientific and Technological Innovations Team of China(2009R50010)
基金supported by the Strategic Priority Research Program of the CAS (No.XDB20000000)the National Natural Science Foundation of China (Nos.U1805252, 21771185,21804134, 51672272, and 21771178)the CAS/SAFEA International Partnership Program for Creative Research Teams, and Natural Science Foundation of Fujian Province (No.201710018).
文摘CuInS2 semiconductor nanocrystals (NCs) exhibit large absorption coefficient, size-dependent photoluminescence and low toxicity, making them excellent candidates in a variety of bioapplications. However, precise control of both their composition and morphology to improve the luminescent efficiency remains a great challenge via conventional direct synthesis. Herein, we present a novel low-temperature template synthesis of highly efficient luminescent CuInS2 nanoprobes from In2S3 NCs via a facile cation exchange strategy. The proposed strategy enables synthesis of a series of CuInS2 NCs with broad size tunability from 2.2 to 29.6 nm. Through rationally manipulating the stoichiometry of Cu/In, highly efficient luminescence of CuInS2 with the maximum quantum yield of 28.6% has been achieved, which is about one order of magnitude improvement relative to that of directly synthesized NCs. By virtue of the intense emission of CuInS2 nanoprobes, we exemplify their application in sensitive homogeneous biodetection for an important biomolecule of adenosine triphosphate (ATP) with the limit of detection down to 49.3 nM. Moreover, the CuInS2 nanoprobes are explored for ATP-targeted cancer cell imaging, thus revealing their great potentials in the field of cancer diagnosis and prognosis.
基金This work was financially supported by the Joint Foundation of National Natural Science Foundation of China(No.U1764254)321 Talent Project of Nanjing,China(No.631783)and 111 Project,China(No.D17003)
文摘Crystal phase engineering on CulnS2(CIS)nanocrystals,especially polytypic structure,has become one of the research hotspots to design the advanced materials and devices for energy conversion and environment treatment.Here,the polytypic CIS nanosheets(NSs)including zincblende/wutzite and chalcopyrite/wurtzite types were first time achieved in a hot-injection system using oleic acid and liquid paraffin as the reaction media.As-obtained polytypic CIS NSs exhibit significantly enhanced light-absorption abillty and visible-light-driven photocatalytic performance originating from the rational hetero-crystalline interfaces and surface defect states,which efficiently inhibit the recombination of photo-generated carriers.Meanwhile,the polytypic CIS NSs were spin-coated onto the surface of fluorinated-tin oxide glass substrate and used as the photoelectrode,which shows an excellent photoelectrochemical(PEC)activity in aqueous solution.The present work not only provides a facile,rapid,low-cost,and environmental-friendly synthesis strategy to design the crystal phase and defect structure of ternary chalcogenides,but also demonstrates the relationships between the polytypic structure and photocatalytic/photoelectrochemical properties.
基金This work was supported in part by the National Key R&D Program of China(2017YFA0207301)the National Natural Science Foundation of China(21725102,U1832156,91961106)+6 种基金CAS Key Research Program of Frontier Sciences(QYZDB-SSW-SLH018)CAS Interdisciplinary Innovation Team,Youth Innovation Promotion Association of CAS(2019444)Science and Technological Fund of Anhui Province for Outstanding Youth(2008085J05)Chinese Academy of Sciences President’s International Fellowship Initiative(2019PC0114)China Postdoctoral Science Foundation(2019M652190)Young Elite Scientist Sponsorship Program by CAST,and DNL Cooperation Fund,CAS(DNL201922)We thank the support from USTC Center for Micro-and Nanoscale Research and Fabrication.
文摘The sharp rise of CO2 in the atmosphere has become a potential threat to global climate, which results from the massive utilization of fossil fuel since the industry revolution. CO2 electroreduction provides us a new possibility of utilizing CO2 as a carbon feedstock for fuel and commercial chemicals generation. In this article, a new method is developed for synthesizing CuInS2 hollow nanostructures through the Kirkendall effect. The CuInS2 hollow nanostructures exhibit excellent catalytic activity for electrochemical reduction of CO2 with particular high selectivity, achieving high faradaic efficiency for HCOOH of 72.8% at -0.7 V. To elucidate the mechanisms, operando electrochemical Raman spectroscopy is employed to examine the CO2 reduction process. This work provides new insights into the design of hollow nanostructures toward electrocatalytic CO2 conversion and offers us an effective and reliable way for real-time investigation of electrochemical CO2 reduction reaction processes.
