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ligand modulation of active center to promote lead-free Cs2AgInCl6 photocatalytic CO2 reduction

Journal of Energy Chemistry 2024年第8期95卷 660-669页

作者： Baofei Sun Wei Chen Yanyi Huang Daofu Wu Heng Luo Faguang Kuang Hongmei Ran Yichen Liu Liqin Gao Jinchen Zhou Bo Gao Qiang Huang Xiaosheng Tang Key Laboratory of Human Brain Bank for Functions and Diseases of Department of Education of Guizhou Province College of Basic Medical Guizhou Medical University College of Optoelectronic Engineering Chongqing University of Posts and Telecommunications School of Electromechanical and Automotive Engineering Yantai University State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Key Laboratory of Optoelectronic Technology & SystemsMinistry of Education College of Optoelectronic Engineering Chongqing University Key Laboratory of Optoelectronic Technology & Systems(Ministry of Education) College of Optoelectronic Engineering Chongqing University School of Materials Science and Engineering Zhengzhou University

Metal halide perovskites（MHP） are potential candidates for the photocatalytic reduction of CO2due to their long photogenerated carrier lifetime and charge diffusion length.However,the conventional long-chain ligand impedes the adsorption and activation of CO2molecules in practical applications.Here,a ligand modulation technology is employed to enhance the photocatalytic CO2reduction activity of lead-free Cs2AgInCl6microcrystals（MCs）.The Cs2AgInCl6MCs passivated by Oleic acid（OLA） and Octanoic acid（OCA） are used for photocatalytic CO2reduction.The results show that the surface defects and electronic properties of Cs2AgInCl6MCs can be adjusted through ligand modulation.Compared with the OLA-Cs2AgInCl6,the OCA-Cs2AgInCl6catalyst demonstrated a significant improvement in the catalytic yield of CO and CH4.The CO and CH4catalytic yields of OCA-Cs2AgInCl6reached 171.88 and34.15 μmol g-1h-1which were 2.03 and 12.98 times higher than those of OLA-Cs2AgInCl6,and the total electron consumption rate of OCA-Cs2AgInCl6was 615.2 μmol g-1h-1which was 3.25 times higher than that of OLA-Cs2AgInCl6.Furthermore,in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs2AgInCl6MCs induced by ligand modulation.This study illustrates the potential of lead-free Cs2AgInCl6MCs for efficient photocatalytic CO2reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts.

关键词： Lead-free perovskite Photocatalysis CO2 reduction Reactive mechanism surface ligand

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The modification toward excited-state dynamics and catalytic activity by isomeric Au_(44)clusters

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Nano Research 2023年第8期16卷 11383-11388页

作者： Tongxin Song Jie Kong Shisi Tang Xiao Cai Xu Liu Meng Zhou Wen Wu Xu Weiping Ding Yan Zhu School of Chemistry and Chemical Engineering Nanjing UniversityNanjing 210093China Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China School of Physical Science and Technology Ningbo UniversityNingbo 315211China

The structure determination of metal nanoclusters protected by ligands is critical in understanding their physical and chemical properties,yet it remains elusive how the metal core and ligand of metal clusters cooperatively contribute to the observed performances.Here,with the successful synthesis of Au_(44)TBPA_(22)Cl_(2)cluster(TBPA=4-tert-butylphenylacetylene),the structural isomer of previously reported Au_(44)L_(28)clusters(L denoted as ligand)is filled,thereby providing an opportunity to explore the property evolution rules imparted by different metal core structures or different surface ligands.Time-resolved transient absorption spectroscopy reveals that the difference in the core structure between Au_(44)TBPA_(22)Cl_(2)and Au_(44)L_(28)can bring nearly 360 times variation of excited-state lifetime,while only 3–24 times differences in excited-state lifetimes of the three Au_(44)L_(28)nanoclusters with identical metal core but different ligands are observed,which is due to much stronger impact of the metal core than the surface ligands in the electronic energy bands of the clusters.In addition,the Au_(44)clusters protected by alkyne ligands are shown to be highly effective toward the electrochemical oxidation of ethanol,compared to the Au_(44)clusters capped by thiolates,which is ascribed to smaller charge transfer impedance of the former clusters.We anticipate that the study will enhance the process in controlling the nanomaterial properties by precisely tailoring metal core or surface patterns.

关键词： cluster metal core surface ligand excited-state dynamics catalysis

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AgAuSe quantum dots with absolute photoluminescence quantum yield of 87.2%:The effect of capping ligand chain length

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Nano Research 2022年第9期15卷 8555-8563页

作者： Ziqiang Sun Cheng Liu Hongchao Yang Xiaohu Yang Yejun Zhang Hongzhen Lin Youyong Li Qiangbin Wang School of Nano-Tech and Nano-Bionics University of Science and Technology of ChinaHefei 230026China CAS Key Laboratory of Nano-Bio Interface Division of Nanobiomedicine and i-LabSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China

surface ligands of colloidal quantum dots(QDs)have a profound influence on their surface states,which has been verified in the studies of the effect of ligand head groups on the photoluminescence(PL)properties of QDs.However,the investigation of the ligand chain length is limited.Here,we systematically explored the effect of chain length on the Ag_(2)Se QDs by selecting three ligands,1-octanethiol(OTT),1-dodecanethiol(DDT),and 1-hexadecanethiol(HDT),with diverse chain lengths.We found that the PL intensity of Ag_(2)Se QDs increased with the decrease of the ligand chain length due to the enhanced passivation of surface defects emerging from the robust QD-ligand interface binding affinity and the weaker hydrophobic chain–chain interaction.Subsequently,AgAuSe QDs terminated with OTT were obtained by alloying parent OTT-Ag_(2)Se QDs with Au precursor with a record absolute PL quantum yield(PLQY)of 87.2%at 970 nm,facilitating ultrasensitive in vivo angiography imaging in a nude mouse model.We expect that our finding of the important role of the ligand chain length on the optical properties of QDs will be suggestive to the design and synthesis of high-quality QDs,and also look forward to the clinical applications of the ultra-bright AgAuSe QDs.

关键词： quantum dots surface ligand ligand chain length photoluminescence quantum yield bioimaging

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Importance of ligands on TiO_2 nanocrystals for perovskite solar cells

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Chinese Physics B 2018年第1期27卷 92-97页

作者：赵耀赵怡程周文可伏睿李琪俞大鹏赵清 State Key Laboratory for Mesoscopic Physics and Electron Microscopy Laboratory School of Physics Peking University

The fabrication of high-quality electron-selective layers at low temperature is a prerequisite to realizing efficient flexible and tandem perovskite solar cells （PSCs）. A colloidal-quantum-dot ink that contains TiO2 nanocrystals enables the deposition of a flat film with matched energy level for PSCs; however, the selection of ligands on the TiO2 surface is still unexplored. Here, we systematically studied the effect of the titanium diisopropoxide bis（acetylacetonate）（TiAc2） ligand on the performance of PSCs with a planar n-i-p architecture. We prepared TiO2 nanocrystals from TiCI4 and ethyl alcohol with C1- ligands attached on its surface and we found that a tiny amount of TiAc2 treatment of as-prepared TiO2 nanocrystals in a mixed solution of chloroform and methyl alcohol can enhance PSC power conversion efficiency （PCE） from 14.7% to 18.3%. To investigate the effect of TiAc2 ligand on PSCs, TiO2 samples with different TiAc2 content were prepared by adding TiAc2 into the as-obtained TiO2 nanocrystal solution. We use x-ray photoelectron spectroscopy to identify the content of C1 so as to reveal that C1 ligands can be substituted by TiAc2. We speculate that the improvement in PCE originates from amorphous TiO2 formation on the TiO2 nanocrystal surface, whereby a single-molecule layer of amorphous TiO2 facilitates charge transfer between the perovskite film and the TiO2 electronic transport layer, but excessive TiAc2 lowers the PSC performance dramatically. We further prove our hypothesis by x-ray diffraction measurements. We believe the PCE of PSCs can be further improved by carefully choosing the type and changing the content of surface ligands on TiO2 nanocrystal.

关键词： TiAc2 TiO2 nanocrystal surface ligand perovskite solar cells

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