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53. Is the kernel–staples match a key–lock match?

Author

Zhuang, Shengli, primary, Liao, Lingwen, additional, Zhao, Yan, additional, Yuan, Jinyun, additional, Yao, Chuanhao, additional, Liu, Xu, additional, Li, Jin, additional, Deng, Haiteng, additional, Yang, Jinlong, additional, and Wu, Zhikun, additional

Published
2018
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56. Gold-Doping of Double-Crown Pd Nanoclusters

Author

Chen, Jishi, primary, Liu, Liren, additional, Liu, Xu, additional, Liao, Lingwen, additional, Zhuang, Shengli, additional, Zhou, Shiming, additional, Yang, Jinlong, additional, and Wu, Zhikun, additional

Published
2017
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58. Quasi‐Dual‐Packed‐Kerneled Au 49 (2,4‐DMBT) 27 Nanoclusters and the Influence of Kernel Packing on the Electrochemical Gap

Author

Liao, Lingwen, primary, Zhuang, Shengli, additional, Wang, Pu, additional, Xu, Yanan, additional, Yan, Nan, additional, Dong, Hongwei, additional, Wang, Chengming, additional, Zhao, Yan, additional, Xia, Nan, additional, Li, Jin, additional, Deng, Haiteng, additional, Pei, Yong, additional, Tian, Shi‐Kai, additional, and Wu, Zhikun, additional

Published
2017
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59. Alternating Array Stacking of Ag26Au and Ag24Au Nanoclusters.

Author

He, Lizhong, Gan, Zibao, Xia, Nan, Liao, Lingwen, and Wu, Zhikun

Subjects
IONS, METALS
Abstract

An assembly strategy for metal nanoclusters using electrostatic interactions with weak interactions, such as C−H⋅⋅⋅π and π⋅⋅⋅π interactions in which cationic [Ag26Au(2‐EBT)18(PPh3)6]+ and anionic [Ag24Au(2‐EBT)18]− nanoclusters gather and assemble in an unusual alternating array stacking structure is presented. [Ag26Au(2‐EBT)18(PPh3)6]+ [Ag24Au(2‐EBT)18]− is a new compound type, a double nanocluster ion compound (DNIC). A single nanocluster ion compound (SNIC) [PPh4]+ [Ag24Au(2‐EBT)18]− was also synthesized, having a k‐vector‐differential crystallographic arrangement. [PPh4]+ [Ag24Au(2,4‐DMBT)18]− adopts a different assembly mode from both [Ag26Au(2‐EBT)18(PPh3)6]+ [Ag24Au(2‐EBT)18]− and [PPh4]+ [Ag24Au(2‐EBT)18]−. Thus, the striking packing differences of [Ag26Au(2‐EBT)18(PPh3)6]+ [Ag24Au(2‐EBT)18]−, [PPh4]+ [Ag24Au(2‐EBT)18]− and the existing [PPh4]+ [Ag24Au(2,4‐DMBT)18]− from each other indicate the notable influence of ligands and counterions on the self‐assembly of nanoclusters. [ABSTRACT FROM AUTHOR]

Published
2019
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62. The fcc structure isomerization in gold nanoclusters

Author

Zhuang, Shengli, primary, Liao, Lingwen, additional, Li, Man-Bo, additional, Yao, Chuanhao, additional, Zhao, Yan, additional, Dong, Hongwei, additional, Li, Jin, additional, Deng, Haiteng, additional, Li, Lingling, additional, and Wu, Zhikun, additional

Published
2017
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65. Fluorescent Gold Nanoclusters with Interlocked Staples and a Fully Thiolate‐Bound Kernel

Author

Gan, Zibao, primary, Lin, Yuejian, additional, Luo, Lun, additional, Han, Guangmei, additional, Liu, Wei, additional, Liu, Zhengjie, additional, Yao, Chuanhao, additional, Weng, Linhong, additional, Liao, Lingwen, additional, Chen, Jishi, additional, Liu, Xu, additional, Luo, Yi, additional, Wang, Chengming, additional, Wei, Shiqiang, additional, and Wu, Zhikun, additional

Published
2016
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68. A Dual Purpose Strategy to Endow Gold Nanoclusters with Both Catalysis Activity and Water Solubility

Author

Zhao, Yan, Zhuang, Shengli, Liao, Lingwen, Wang, Chengming, Xia, Nan, Gan, Zibao, Gu, Wanmiao, Li, Jin, Deng, Haiteng, and Wu, Zhikun

Abstract

Gold nanoclusters have attracted extensive interest for catalysis applications in recent years due to their ultrasmall sizes and well-defined compositions and structures. However, at least two challenges exist in this emerging field. First, the steric hindrance of the ligands inhibits the catalysis activity, and second, the mechanism underlying water-phase catalysis using gold nanoclusters is often ambiguous. Herein, we introduce a “kill two birds with one stone” strategy to address these two challenges via the use of host–guest chemistry. As an illustration, a novel adamantanethiolate-protected Au40(S-Adm)22nanocluster was synthesized, bound with γ-CD-MOF, and then transferred to the HRP-mimicking reaction system. The as-obtained catalyst exhibits excellent water solubility and catalytical activity, totally different from the virgin Au40(S-Adm)22nanoclusters. Further, the detailed HRP-mimicking catalysis mechanism was proposed and supported by DFT calculation. Another interesting finding is the unique structure of Au40(S-Adm)22, which can be regarded as an Au13icosahedron unit derived structure but different from the widely reported icosahedron contained nanocluster where the Au13icosahedrons are often centered. These novel, intriguing results have important implication for the property tuning and practical application of metal nanoclusters in the future.

Published
2020
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69. Bimetal Doping in Nanoclusters: Synergistic or Counteractive?

Author

Yan, Nan, Liao, Lingwen, Yuan, Jinyun, Lin, Yue-jian, Weng, Lin-hong, Yang, Jinlong, and Wu, Zhikun

Abstract

Doped nanoparticles (especially bimetal doped nanoparticles) have attracted extensive interest not only for fundamental scientific research but also for application purposes. However, their indefinite composition (structure) and broad distribution hinder an insightful understanding of the interaction between these invasive metals in bimetal doped nanoparticles. Fortunately, atom-precise bimetal doped ultrasmall nanoparticles (nanoclusters) provide opportunities to obtain such insights. However, atom-precise trimetal nanoclusters and their structures have rarely been reported. Here, we successfully dope thiolated Au25nanoclusters with Hg and Ag successively by using a biantigalvanic reduction method. We then fully characterize the as-obtained trimetal nanoclusters using multiple techniques (including single-crystal X-ray crystallography), and we demonstrate that the mercury and silver dopings exhibit not only a synergistic but also a counteractive influence on some of the physicochemical properties of Au25.

Published
2024
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75. Quasi-Dual-Packed-Kerneled Au49(2,4-DMBT)27 Nanoclusters and the Influence of Kernel Packing on the Electrochemical Gap.

Author

Liao, Lingwen, Zhuang, Shengli, Wang, Pu, Xu, Yanan, Yan, Nan, Dong, Hongwei, Wang, Chengming, Zhao, Yan, Xia, Nan, Li, Jin, Deng, Haiteng, Pei, Yong, Tian, Shi ‐ Kai, and Wu, Zhikun

Subjects
*GOLD nanoparticles, *ELECTROCHEMISTRY, *BODY-centered cubic metals, *CRYSTAL structure, *ELECTRONIC structure
Abstract

Although face-centered cubic (fcc), body-centered cubic (bcc), hexagonal close-packed (hcp), and other structured gold nanoclusters have been reported, it was unclear whether gold nanoclusters with mix-packed (fcc and non-fcc) kernels exist, and the correlation between kernel packing and the properties of gold nanoclusters is unknown. A Au49(2,4-DMBT)27 nanocluster with a shell electron count of 22 has now been been synthesized and structurally resolved by single-crystal X-ray crystallography, which revealed that Au49(2,4-DMBT)27 contains a unique Au34 kernel consisting of one quasi-fcc-structured Au21 and one non-fcc-structured Au13 unit (where 2,4-DMBTH=2,4-dimethylbenzenethiol). Further experiments revealed that the kernel packing greatly influences the electrochemical gap (EG) and the fcc structure has a larger EG than the investigated non-fcc structure. [ABSTRACT FROM AUTHOR]

Published
2017
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81. Transition-sized Au92 nanoparticle bridging non-fcc-structured gold nanoclusters and fcc-structured gold nanocrystals.

Author

Liao, Lingwen, Chen, Jishi, Wang, Chengming, Zhuang, Shengli, Yan, Nan, Yao, Chuanhao, Xia, Nan, Li, Lingling, Bao, Xiaoli, and Wu, Zhikun

Subjects
*LIGHT absorption, *ELECTROCHEMISTRY, *NANOPARTICLES, *UNIT cell, *SINGLE crystals
Abstract

Herein, we report the intriguing structure, optical absorption and electrochemical properties of the transition-sized Au92(TBBT)44 (Au92 for short, TBBT = 4-tert-butylbenzenethiolate) nanoparticle. An interesting observation is the 4H phase array of Au92 nanoparticles in the unit cells of single crystals. [ABSTRACT FROM AUTHOR]

Published
2016
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82. Structures and magnetism of mono-palladium and mono-platinum doped Au25(PET)18 nanoclusters.

Author

Tian, Shubo, Liao, Lingwen, Yuan, Jinyun, Yao, Chuanhao, Chen, Jishi, Yang, Jinlong, and Wu, Zhikun

Subjects
*PALLADIUM, *PLATINUM, *CRYSTAL structure, *MAGNETIC structure, *DOPED semiconductors, *CATALYSIS
Abstract

Herein we report three important results of widespread interest, which are (1) the crystal structure of [Au24Pt(PET)18]0, (2) the crystal structure of [Au24Pd(PET)18]0 and (3) the main source of magnetism in [Au25(PET)18]0. [ABSTRACT FROM AUTHOR]

Published
2016
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87. Chemical Synthesis of ~1 nm Multilevel Capacitor‐like Particles with Atomic Precision.

Author

Zhou, Yue, Chen, Dong, Gu, Wanmiao, Fan, Wentao, Wang, Runguo, Fang, Liang, You, Qing, Zhuang, Shengli, Bian, Guoqing, Liao, Lingwen, Zhou, Ziyan, Xia, Nan, Yang, Jun, and Wu, Zhikun

Subjects
*METAL nanoparticles, *NANOPARTICLES, *CHEMICAL synthesis, *SLEEVES, *VOLTAMMETRY
Abstract

Can the chemically synthesized nanoparticles act as nanodevices or nanomachines? Herein, we demonstrated this feasibility. A novel nanocluster (ultrasmall nanoparticle) [Au44Cd20(m‐MBT)40][N(C8H17)4]2 (Au44Cd20 in short, m‐MBTH: m‐methylbenzenethiol) obtained via developing a synthesis method has a cannula‐like structure of the outer shell and an internal sleeve, revealed by single‐crystal X‐ray diffraction. Natural population analysis (NPA) charge calculations, charge carrier transport of Au44Cd20 (during which an intra‐nanocluster anti‐galvanic reaction was observed) after unneutral charging using NaBH4 as well as voltammetry proved the capacitor‐like character of Au44Cd20. The subsidiary capacitor‐like character of the outer shell of Au44Cd20 was further probed via NPA charge calculations and electrocatalytic reduction of CO2 to CO. Thus, this study predicts a new era of engineering metal nanoparticles for realizing atomically precise ultrasmall nanodevices and nanomachines. [ABSTRACT FROM AUTHOR]

Published
2024
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88. Gapped and Rotated Grain Boundary Revealed in Ultra‐Small Au Nanoparticles for Enhancing Electrochemical CO2 Reduction.

Author

Wang, Wenying, Chen, Dong, Fung, Victor, Zhuang, Shengli, Zhou, Yue, Wang, Chengming, Bian, Guoqing, Zhao, Yan, Xia, Nan, Li, Jin, Deng, Haiteng, Liao, Lingwen, Yang, Jun, Jiang, De‐en, and Wu, Zhikun

Abstract

Although gapped grain boundaries have often been observed in bulk and nanosized materials, and their crucial roles in some physical and chemical processes have been confirmed, their acquisition at ultrasmall nanoscale presents a significant challenge. To date, they had not been reported in metal nanoparticles smaller than 2 nm owing to the difficulty in characterization and the high instability of grain boundary (GB) atoms. Herein, we have successfully developed a synthesis method for producing a novel chiral nanocluster Au78(TBBT)40 (TBBT=4‐tert‐butylphenylthiolate) with a 26‐atom gapped and rotated GB. This nanocluster was precisely characterized using single‐crystal X‐ray crystallography and mass spectrometry. Additionally, an offset atomic defect linked to the peripheral Au(TBBT)2 staple was found in the structure. Comparing it to similarly face‐centered cubic‐structured Au36(TBBT)24, Au44(TBBT)28, Au52(TBBT)32, Au92(TBBT)44, and ~5 nm nanocrystals, the bridging Au78(TBBT)40 nanocluster exhibited higher catalytic activity in the electroreduction of CO2 to CO. This enhanced activity was explained through density functional theory calculations and X‐ray photoelectron spectroscopy analysis, which highlight the impact of GBs and point defects on the surface properties of metal nanoclusters in balancing intermediate adsorption and product desorption. [ABSTRACT FROM AUTHOR]

Published
2024
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89. Preparation of Au@Pd Core–Shell Nanorods with fcc-2H-fccHeterophase for Highly Efficient Electrocatalytic Alcohol Oxidation

Author

Zhou, Xichen, Ma, Yangbo, Ge, Yiyao, Zhu, Shangqian, Cui, Yu, Chen, Bo, Liao, Lingwen, Yun, Qinbai, He, Zhen, Long, Huiwu, Li, Lujiang, Huang, Biao, Luo, Qinxin, Zhai, Li, Wang, Xixi, Bai, Licheng, Wang, Gang, Guan, Zhiqiang, Chen, Ye, Lee, Chun-Sing, Wang, Jinlan, Ling, Chongyi, Shao, Minhua, Fan, Zhanxi, and Zhang, Hua

Abstract

Controlled construction of bimetallic nanostructures with a well-defined heterophase is of great significance for developing highly efficient nanocatalysts and investigating the structure-dependent catalytic performance. Here, a wet-chemical synthesis method is used to prepare Au@Pd core–shell nanorods with a unique fcc-2H-fccheterophase (fcc: face-centered cubic; 2H: hexagonal close-packed with a stacking sequence of “AB”). The obtained fcc-2H-fccheterophase Au@Pd core–shell nanorods exhibit superior electrocatalytic ethanol oxidation performance with a mass activity as high as 6.82 A mgPd–1, which is 2.44, 6.96, and 6.43 times those of 2H-Pd nanoparticles, fcc-Pd nanoparticles, and commercial Pd/C, respectively. The operandoinfrared reflection absorption spectroscopy reveals a C2 pathway with fast reaction kinetics for the ethanol oxidation on the prepared heterophase Au@Pd nanorods. Our experimental results together with density functional theory calculations indicate that the enhanced performance of heterophase Au@Pd nanorods can be attributed to the unconventional 2H phase, the 2H/fccphase boundary, and the lattice expansion of the Pd shell. Moreover, the heterophase Au@Pd nanorods can also serve as an efficient catalyst for the electrochemical oxidation of methanol, ethylene glycol, and glycerol. Our work in the area of phase engineering of nanomaterials (PENs) opens the way for developing high-performance electrocatalysts toward future practical applications.

Published
2021
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90. Inside Back Cover: Gapped and Rotated Grain Boundary Revealed in Ultra‐small Au Nanoparticles for Enhancing Electrochemical CO2 Reduction.

Author

Wang, Wenying, Chen, Dong, Fung, Victor, Zhuang, Shengli, Zhou, Yue, Wang, Chengming, Bian, Guoqing, Zhao, Yan, Xia, Nan, Li, Jin, Deng, Haiteng, Liao, Lingwen, Yang, Jun, Jiang, De‐en, and Wu, Zhikun

Subjects
*GOLD nanoparticles, *CRYSTAL grain boundaries, *METAL nanoparticles, *ELECTROLYTIC reduction, *NANOPARTICLES
Abstract

Although gapped grain boundaries have often been observed in bulk and nanosized materials, theyhave not been reported in metal nanoparticles smaller than 2 nm owing to the difficulty in characterization and the high instability of grain boundary ( GB) atoms. In their Research Article ( e202410109), Zhikun Wu, Jun Yang, Lingwen Liao et al. report a novel nanocluster with a 26- atom gapped and rotated GB, and demonstrate the effectiveness of manipulating GBs for enhancing the catalytic activity of nanocatalysts. [Extracted from the article]

Published
2024
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