Atomically precise bimetallic metal ensembles with tailorable synergistic effects

Tianxiang Chen; Yong Wang; Qi Xue; Ching Kit Tommy Wun; Pui Kin So; Ka Fu Yung; Tai-Sing Wu; Yun-Liang Soo; Keita Taniya; Sarah Day; Chiu C. Tang; Zehao Li; Bolong Huang; Shik Chi Edman Tsang; Kwok-yin Wong; Tsz Woon Benedict Lo

doi:10.1016/j.xcrp.2022.100850

Atomically precise bimetallic metal ensembles with tailorable synergistic effects

Tianxiang Chen, Yong Wang, Qi Xue, Ching Kit Tommy Wun, Pui Kin So, Ka Fu Yung, Tai-Sing Wu, Yun-Liang Soo, Keita Taniya, Sarah Day, Chiu C. Tang, Zehao Li, Bolong Huang^*, Shik Chi Edman Tsang, Kwok-yin Wong^*, Tsz Woon Benedict Lo^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

9 Citations (Scopus)

13 Downloads (CityUHK Scholars)

Abstract

The large-scale synthesis of supported multinuclear catalysts with controllable metal nuclearity and constituent composition remains a formidable challenge. We report the stepwise assembly of supported atom-precise bimetallic ligand-mediated metal ensembles (LMMEs) by exploiting the underlying principles of coordination chemistry and solid-state chemistry. Lewis di-basic 2-methylimidazole is used to bridge multiple Cu²⁺ and M²⁺ (M = Co, Ni, Cu, and Zn) ions within ZSM-5 zeolites. We observe the metal constituent composition of the LMMEs by mass spectroscopy. The adjacent metal nuclei in the LMMEs offer substantial synergistic effects that enhance the catalytic performance by at least an order of magnitude in the model catalytic “click” reaction. It is envisaged that this stepwise assembly approach to develop supported multinuclear catalysts with atom precision could effectively bridge homogeneous and heterogeneous catalysis. © 2022 The Author(s).

Original language	English
Article number	100850
Journal	Cell Reports Physical Science
Volume	3
Issue number	4
Online published	8 Apr 2022
DOIs	https://doi.org/10.1016/j.xcrp.2022.100850
Publication status	Published - 20 Apr 2022
Externally published	Yes

Funding

We thank Diamond Light Source, SPring-8, and NSRRC for the provision of valuable synchrotron beamtime for SXRD and EXAFS measurements (CY26404 2020A1088 and 2020A0565). This work was supported by the Hong Kong Research Grants Council (15301521 and 15300819) and the National Natural Science Foundation of China (22172136) for financial support (T.W.B.L.). Finally, we thank UMF, UCEA, and UMF of PolyU for their support in materials characterization.

Research Keywords

bimetallic catalysts
binuclear metal ensembles
dual-atoms
MALDI-MS characterization
microporous supports
modular assembly
precise control
structural refinements
synergistic effects
“click” reaction

Publisher's Copyright Statement

This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

RGC Funding Information

RGC-funded

Access Output

10.1016/j.xcrp.2022.100850

268435732.pdfFinal Published version, 3.44 MBLicence: CC BY

Other Access Options

Check CityUHK Library

Permanent Link

Right click to copy link

Cite this

Chen, T., Wang, Y., Xue, Q., Wun, C. K. T., So, P. K., Yung, K. F., Wu, T.-S., Soo, Y.-L., Taniya, K., Day, S., Tang, C. C., Li, Z., Huang, B., Tsang, S. C. E., Wong, K., & Lo, T. W. B. (2022). Atomically precise bimetallic metal ensembles with tailorable synergistic effects. Cell Reports Physical Science, 3(4), Article 100850. https://doi.org/10.1016/j.xcrp.2022.100850

@article{28bb11afe0c04fe2a46b1fd6be0fe899,

title = "Atomically precise bimetallic metal ensembles with tailorable synergistic effects",

abstract = "The large-scale synthesis of supported multinuclear catalysts with controllable metal nuclearity and constituent composition remains a formidable challenge. We report the stepwise assembly of supported atom-precise bimetallic ligand-mediated metal ensembles (LMMEs) by exploiting the underlying principles of coordination chemistry and solid-state chemistry. Lewis di-basic 2-methylimidazole is used to bridge multiple Cu2+ and M2+ (M = Co, Ni, Cu, and Zn) ions within ZSM-5 zeolites. We observe the metal constituent composition of the LMMEs by mass spectroscopy. The adjacent metal nuclei in the LMMEs offer substantial synergistic effects that enhance the catalytic performance by at least an order of magnitude in the model catalytic “click” reaction. It is envisaged that this stepwise assembly approach to develop supported multinuclear catalysts with atom precision could effectively bridge homogeneous and heterogeneous catalysis. {\textcopyright} 2022 The Author(s).",

keywords = "bimetallic catalysts, binuclear metal ensembles, dual-atoms, MALDI-MS characterization, microporous supports, modular assembly, precise control, structural refinements, synergistic effects, “click” reaction",

author = "Tianxiang Chen and Yong Wang and Qi Xue and Wun, {Ching Kit Tommy} and So, {Pui Kin} and Yung, {Ka Fu} and Tai-Sing Wu and Yun-Liang Soo and Keita Taniya and Sarah Day and Tang, {Chiu C.} and Zehao Li and Bolong Huang and Tsang, {Shik Chi Edman} and Kwok-yin Wong and Lo, {Tsz Woon Benedict}",

year = "2022",

month = apr,

day = "20",

doi = "10.1016/j.xcrp.2022.100850",

language = "English",

volume = "3",

number = "4",

}

TY - JOUR

T1 - Atomically precise bimetallic metal ensembles with tailorable synergistic effects

AU - Chen, Tianxiang

AU - Wang, Yong

AU - Xue, Qi

AU - Wun, Ching Kit Tommy

AU - So, Pui Kin

AU - Yung, Ka Fu

AU - Wu, Tai-Sing

AU - Soo, Yun-Liang

AU - Taniya, Keita

AU - Day, Sarah

AU - Tang, Chiu C.

AU - Li, Zehao

AU - Huang, Bolong

AU - Tsang, Shik Chi Edman

AU - Wong, Kwok-yin

AU - Lo, Tsz Woon Benedict

PY - 2022/4/20

Y1 - 2022/4/20

N2 - The large-scale synthesis of supported multinuclear catalysts with controllable metal nuclearity and constituent composition remains a formidable challenge. We report the stepwise assembly of supported atom-precise bimetallic ligand-mediated metal ensembles (LMMEs) by exploiting the underlying principles of coordination chemistry and solid-state chemistry. Lewis di-basic 2-methylimidazole is used to bridge multiple Cu2+ and M2+ (M = Co, Ni, Cu, and Zn) ions within ZSM-5 zeolites. We observe the metal constituent composition of the LMMEs by mass spectroscopy. The adjacent metal nuclei in the LMMEs offer substantial synergistic effects that enhance the catalytic performance by at least an order of magnitude in the model catalytic “click” reaction. It is envisaged that this stepwise assembly approach to develop supported multinuclear catalysts with atom precision could effectively bridge homogeneous and heterogeneous catalysis. © 2022 The Author(s).

AB - The large-scale synthesis of supported multinuclear catalysts with controllable metal nuclearity and constituent composition remains a formidable challenge. We report the stepwise assembly of supported atom-precise bimetallic ligand-mediated metal ensembles (LMMEs) by exploiting the underlying principles of coordination chemistry and solid-state chemistry. Lewis di-basic 2-methylimidazole is used to bridge multiple Cu2+ and M2+ (M = Co, Ni, Cu, and Zn) ions within ZSM-5 zeolites. We observe the metal constituent composition of the LMMEs by mass spectroscopy. The adjacent metal nuclei in the LMMEs offer substantial synergistic effects that enhance the catalytic performance by at least an order of magnitude in the model catalytic “click” reaction. It is envisaged that this stepwise assembly approach to develop supported multinuclear catalysts with atom precision could effectively bridge homogeneous and heterogeneous catalysis. © 2022 The Author(s).

KW - bimetallic catalysts

KW - binuclear metal ensembles

KW - dual-atoms

KW - MALDI-MS characterization

KW - microporous supports

KW - modular assembly

KW - precise control

KW - structural refinements

KW - synergistic effects

KW - “click” reaction

UR - http://www.scopus.com/inward/record.url?scp=85128512906&partnerID=8YFLogxK

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85128512906&origin=recordpage

U2 - 10.1016/j.xcrp.2022.100850

DO - 10.1016/j.xcrp.2022.100850

M3 - RGC 21 - Publication in refereed journal

SN - 2666-3864

VL - 3

JO - Cell Reports Physical Science

JF - Cell Reports Physical Science

IS - 4

M1 - 100850

ER -

Atomically precise bimetallic metal ensembles with tailorable synergistic effects

Abstract

Funding

Research Keywords

Publisher's Copyright Statement

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Cite this