JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Jieding Wei,Renqiang Zhao,Dian Luo,Xiangyu Lu,Wenxiu Dong,Yucheng Huang,Xiaomei Cheng,Yonghong Ni
Much effort has been devoted to improving the photocatalytic capacity of graphitic carbon nitride (g-C 3 N 4 ). In this paper, we reported the successful synthesis of a hybrid photocatalyst with superb photocatalytic hydrogen production activity through decorating atomically precise Ni 6 (SC 2 H 4 Ph) 12 nanoclusters on g-C 3 N 4 nanosheets (labeled as Ni 6 /g-C 3 N 4 ) at room temperature. Zeta potential experiments demonstrated that the electrostatic interaction between Ni 6 and g-C 3 N 4 led to the formation of Ni 6 /g-C 3 N 4 . The photocatalytic measurements revealed that the 5 %-Ni 6 /g-C 3 N 4 prepared with the original mass ratio of m(Ni 6 )/m(g-C 3 N 4 ) = 1/20 exhibited the strongest hydrogen production activity. In the system with triethanolamine (TEOA) as the sacrifice agent, the visible-light hydrogen production rate reached up to 5.87 mmol h −1 g −1 , approximately 290 times higher than that of pure g-C 3 N 4 (0.02 mmol h −1 g −1 ). Density functional theory (DFT) calculations testified that the above significant enhancement of photocatalytic hydrogen evolution of the hybrid photocatalyst arose from the photogenerated electrons transfer from Ni 6 to g-C 3 N 4 .
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高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Xia Nan,Xing Jianpei,Peng Di,Ji Shiyu,Zha Jun,Yan Nan,Su Yan,Jiang Xue,Zeng Zhi,Zhao Jijun,Wu Zhikun
Nanoparticle assembly paves the way for unanticipated properties and applications from the nanoscale to the macroscopic world. However, the study of such material systems is greatly inhibited due to the obscure compositions and structures of nanoparticles (especially the surface structures). The assembly of atomically precise nanoparticles is challenging, and such an assembly of nanoparticles with metal core sizes strictly larger than 1 nm has not been achieved yet. Here, we introduced an on-site synthesis-and-assembly strategy, and successfully obtained a straight-chain assembly structure consisting of Ag 77 Cu 22 (CHT) 48 (CHT: cyclohexanethiolate) nanoparticles with two nanoparticles separated by one S atom, as revealed by mass spectrometry and single crystal X-ray crystallography. Although Ag 77 Cu 22 (CHT) 48 bears one unpaired shell-closing electron, the magnetic moment is found to be mainly localized at the S linker with magnetic isotropy, and the sulfur radicals were experimentally verified and found to be unstable after disassembly, demonstrating assembly-induced spin transfer. Besides, spin nanoparticles are found to couple and lose their paramagnetism at sufficiently short inter-nanoparticle distance, namely, the spin coupling depends on the inter-nanoparticle distance. However, it is not found that the spin coupling leads to the nanoparticle growth.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Jinling Yang,Xiang Li,Jianrong Zhang,Yang Zhou,Yuanyuan Wang
All-inorganic metal nanocrystals (NCs) offer an ideal platform for atomically precise surface design and show improved electrocatalytic activity compared to conventional NCs capped with organic ligands. Here, we show the possibility of obtaining colloidal all-inorganic Au NCs directly from magic-size clusters (MSCs) with the assistance of inorganic molecules, NOBF4 or Na2S2O8. The unique advantages of NOBF4 or Na2S2O8 as both oxidizing agents and stripping ligands are taken to tune the surface state of Au25(PET)18–TOA+ MSCs and assemble them to form either positively or negatively charged all-inorganic Au NCs. We show that positively charged all-inorganic Au NCs can be further modified with different functional groups, which provide the possibility to meet the target requirements. We found that the negatively charged NCs exhibit improved faradaic efficiency (FE = 92%) for the reduction of CO2 to CO at −0.369 V (vs RHE) and a 5-fold increase in current density compared to organic-capped Au NCs (FE = 67%). In addition, we extended this approach to other MSCs and formed all-inorganic metal NCs with different compositions and morphologies. The use of simple inorganic ligands to induce the conversion from MSCs to metal NCs enriches the current solution process of synthesizing all-inorganic NCs and can open up more opportunities for designing colloidal nanocrystal catalysts.
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RSC Advances
·
2021
·Vol. 11
·期 24
·14678-14685
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IF 3.361
Yiling Li,Shuxiao Yi,Zhongli Lei,Yan Xiao
It is of vital importance to develop probes to monitor hypochlorous acid (HClO) in biological systems as HClO is associated with many important physiological and pathological processes. Metal nanoclusters (NCs) are promising luminescent nanomaterials for highly reactive oxygen species (hROS) detection on the basis of their strong reaction ability with hROS. However, metal NCs typically can respond to most common hROS and are susceptible to etching by biothiols, hindering their application in the construction of effective HClO probes. Herein, we proposed a strategy to develop a nanoprobe based on Au NCs for highly sensitive and selective detection of HClO. We synthesized luminescent benzyl mercaptan-stabilized Au NCs and encapsulated them with an amphiphilic polymer (DSPE-PEG). After encapsulation, an obvious emission enhancement and good resistance to the etching by biothiols for Au NCs were achieved. More importantly, the DSPE-PEG encapsulated Au NCs can be used as a nanoprobe for detection of HClO with good performance. The luminescence of the Au NCs was effectively and selectively quenched by HClO. A good linear relationship with the concentration of HClO in the range of 5–35 μM and a limit of detection (LOD) of 1.4 μM were obtained. Additionally, this nanoprobe was successfully used for bioimaging and monitoring of HClO changes in live cells, suggesting the application potential of the as-prepared amphiphilic polymer-encapsulated Au NCs for further HClO-related biomedical research.
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Nature Communications
·
2020
·Vol. 11
·期 1
·1-7
·
IF 12.121
Liu Xu,Xu Wen Wu,Huang Xinyu,Wang Endong,Cai Xiao,Zhao Yue,Li Jin,Xiao Min,Zhang Chunfeng,Gao Yi,Ding Weiping,Zhu Yan
The discovery of atomically precise nanoclusters is generally unpredictable, and the rational synthesis of nanoclusters guided by the theoretical design is still in its infancy. Here we present a de novo design of Au 36 (SR) 24 nanoclusters, from theoretical prediction to experimental synthesis and characterization of their physicochemical properties. The crystal structure of an Au 36 (SR) 24 nanocluster perfectly matches the simulated structural pattern with Au 4 tetrahedral units along a two-dimensional growth. The Au 36 (SR) 24 nanocluster indeed differs from its structural isomer whose kernel is dissected in an Au 4 tetrahedral manner along a one-dimensional growth. The structural isomerism in the Au 36 (SR) 24 nanoclusters further induces distinct differences in ultrafast electron dynamics and chirality. This work will not only promote the atomically precise synthesis of nanoclusters enlightened by theoretical science, but also open up exciting opportunities for underpinning the widespread applications of structural isomers with atomic precision.
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CHEMISTRY OF MATERIALS
·
2018
·
IF 9.89
Yali Liu,Pengfei Zhang,Junmin Liu,Tao Wang,Qisheng Huo,Li Yang,Lei Sun,Zhen-An Qiao,Sheng Dai
Gold clusters with ultrasmall size and special structure are highly attractive for heterogeneous catalysis. However, stabilizing gold clusters under thermal treatment remains a major hurdle on the way toward real-world application. Herein, we report an effective approach that stabilizing gold clusters (Au25 and Au144) within mesoporous ceria nanospheres via a two phase overcoating process. High-resolution aberration-corrected STEM studies indicated that gold clusters were encapsulated and confined in the intersectional channels of ceria, and the encapsulated clusters were demonstrated to be resistant to sintering under high-temperature thermal treatment. The solvent-free aerobic oxidation of toluene and ethylbenzene was carried out to illustrate the performance of gold clusters in catalysis, and these materials showed excellent catalytic activities and afforded much higher turnover frequencies (up to 5634 and 55 027 turnovers for toluene and ethylbenzene oxidation), which are, as far as we know, much higher than the values of state-of-art catalysts. Density functional theory calculations revealed that the encapsulated gold clusters effectively reduced the energy required for the dissociation of O2 molecules, leading to the excellent catalytic activity.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Xu Liu,Jin Tang,Fangming Zhao,Meng Zhou,Siyang Ye,Daocheng Hong,Yuxi Tian,Yue Zhao,Shuangshuang Huang,Fan Tian,Tongxin Song,Xiao Cai,Yiqi Tian,Wei Zhang,Qi Li,Yan Zhu
Precise doping is of vital significance for atomic engineering and the establishment of structure-property relationships in nanocluster (NC) chemistry. Herein, two novel trimetallic MAu 18 Cd 3 (M = Pd/Pt) NCs that are derived from M-doped Au 25 templates of MAu 24 are reported, in which the central doping of M atom and the surface-motif doping of Cd atoms are concurrently achieved. Compared to the original templates, Cd-induced surface engineering enhances the rigidity of the structural framework and enlarges the HOMO-LUMO gaps of the MAu 18 Cd 3 , significantly improving photoluminescent efficiency by suppressing nonradiative relaxation. The critical role of the central M (Pd/Pt) dopant in photoluminescence, which regulates the rate of radiative decay of excited-state electrons, has also been substantiated. More notably, the doped case of PtAu 18 Cd 3 exhibits excellent photoinitiation activity in 3D two-photon printing with a high resolution of ≈140 nm, which may be attributed to the prolonged excited state. Overall, this work provides a generalized routine for the precise synthesis of multi-metal NCs with concurrent enhancements in photoluminescence and photoinitiation activity, which is expected to stimulate further research for the design and preparation of multi-functional, multi-metal NCs.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Dan Yang,Xiang Cui,Zhou Xu,Qian Yan,Yating Wu,Chunmei Zhou,Yihu Dai,Xiaoyue Wan,Yuguang Jin,Leonid M. Kustov,Yanhui Yang
The electrocatalytic oxidation of glycerol toward formic acid is one of the most promising pathways for transformation and utilization of glycerol. Herein, a series of well-defined Ni n (SR) 2 n nanoclusters ( n = 4, 5, 6; denoted as Ni NCs) were prepared for the electrocatalytic glycerol oxidation toward formic acid, in which Ni 6 -PET-50CV afforded the most excellent electrocatalytic performance with a high formic acid selectivity of 93% and a high glycerol conversion of 86%. This was attributed to the lowest charge transfer impedance and the most rapid reaction kinetics. Combined electrochemical measurements and X-ray absorption fine structure measurements revealed that the structures of Ni NCs remained intact after CV scanning pretreatment and electrocatalysis via forming the Ni–O bond. Additionally, the kinetic studies and in-situ Fourier transformed infrared suggested a sequential oxidation mechanism, in which the main reaction steps of glycerol → glyceraldehyde → glyceric acid were very rapid to produce a high selectivity of formic acid even though the low glycerol conversion. This work presents an opportunity to study Ni NCs for the efficient electrocatalytic oxidation of biomass-derived polyhydroxyl platform molecules to produce value-added carboxylic acids.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Xu Guangyuan,Peng Xingjie,Wu Chuanqiang,Xi Shibo,Xiang Huixin,Feng Lei,Liu Zhendong,Duan Yi,Gan Lijin,Chen Si,Kong Yuan,Ma Yanzhe,Nie Fujing,Zhao Jie,Hai Xiao,Wei Wei,Zhou Meng,Wang Tianfu,Yao Chuanhao,Zhou Wu,Yan Huan
CO 2 electroreduction to CO promises to give an efficient strategy for CO 2 fixation and transformation. However, current reported active sites fail to deliver sufficient activity with high CO Faradic efficiency (FEco) over a wide range of potential. Here, we show a general synthetic protocol to fabricate a batch of highly pure and active NiN 2 catalysts with precise engineering of the uniform-large ( UL ) vacancy around the active sites, which is accomplished through the ‘pre-deposition + pyrolysis’ of various atomically precise Ni clusters (Ni n ) and in-situ etching of the support by the ‘nano bomb’ (sulfur-ligand in the clusters). The NiN 2 sites with UL vacancies could achieve a high turnover frequency (TOF) of 350000 h −1 with ~100% FEco in a wide potential range of 1500 mV. In-situ infrared spectra and theoretical calculations reveal that a highly pure NiN 2 site with UL vacancy contributes to this remarkable catalytic performance compared to the counterparts. This general synthetic strategy enables us to simultaneously engineer active sites and surrounding vacancies with the employment of atomically precise metal clusters, thereby enhancing catalytic performance for other specific reactions.
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