2024
|
Guo, Shasha; Zhou, Xiuxian; Lee, Jinn-kye; Guo, Qing; Liu, Xiao; Wu, Yao; Ma, Mingyu; Zhang, Zhengyang; Liu, Zheng Nanoscale Identification of Local Strain Effect on TMD Catalysis JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2024, DOI: 10.1021/jacs.4c11190. Abstract | BibTeX | Endnote @article{ISI:001351705600001,
title = {Nanoscale Identification of Local Strain Effect on TMD Catalysis},
author = {Shasha Guo and Xiuxian Zhou and Jinn-kye Lee and Qing Guo and Xiao Liu and Yao Wu and Mingyu Ma and Zhengyang Zhang and Zheng Liu},
doi = {10.1021/jacs.4c11190},
times_cited = {0},
issn = {0002-7863},
year = {2024},
date = {2024-11-08},
journal = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Strain engineering plays a crucial role in activating the basal plane of the TMD catalysts. However, experimental evidence linking strain strength to activity and distinguishing effects of compressive and tensile strain remains elusive due to the absence of high-resolution in situ correlation techniques. Here, we utilize nanobubble imaging by on-chip total-internal reflection microscopy to visualize active sites on the basal plane of strained MoS2 during hydrogen evolution reaction and atomic force microscopy to correlatively capture the nanoscale morphology and strain maps. By integrating the activity, morphology, and strain maps into comprehensive statistical analyses, we elucidate the strain effect on local activity at both multiprotrusion and (sub)single-protrusion levels. Our findings demonstrate that strain effectively activates sulfur vacancies on the basal plane, with tensile strain significantly enhancing local activity compared to compressive strain. Furthermore, we observe a time-dependent propagation of activity from high-activity to low-activity regions within single protrusions. This work clarifies the interplay between structural morphology and catalytic activity and provides new guidelines for the rational design of optimal TMD catalysts.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Strain engineering plays a crucial role in activating the basal plane of the TMD catalysts. However, experimental evidence linking strain strength to activity and distinguishing effects of compressive and tensile strain remains elusive due to the absence of high-resolution in situ correlation techniques. Here, we utilize nanobubble imaging by on-chip total-internal reflection microscopy to visualize active sites on the basal plane of strained MoS2 during hydrogen evolution reaction and atomic force microscopy to correlatively capture the nanoscale morphology and strain maps. By integrating the activity, morphology, and strain maps into comprehensive statistical analyses, we elucidate the strain effect on local activity at both multiprotrusion and (sub)single-protrusion levels. Our findings demonstrate that strain effectively activates sulfur vacancies on the basal plane, with tensile strain significantly enhancing local activity compared to compressive strain. Furthermore, we observe a time-dependent propagation of activity from high-activity to low-activity regions within single protrusions. This work clarifies the interplay between structural morphology and catalytic activity and provides new guidelines for the rational design of optimal TMD catalysts. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUGuo, SS
Zhou, XX
Lee, JK
Guo, Q
Liu, X
Wu, Y
Ma, MY
Zhang, ZY
Liu, Z
- AFShasha Guo
Xiuxian Zhou
Jinn-kye Lee
Qing Guo
Xiao Liu
Yao Wu
Mingyu Ma
Zhengyang Zhang
Zheng Liu
- TINanoscale Identification of Local Strain Effect on TMD Catalysis
- SOJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
- LAEnglish
- DTArticle
- IDMOS2
- ABStrain engineering plays a crucial role in activating the basal plane of the TMD catalysts. However, experimental evidence linking strain strength to activity and distinguishing effects of compressive and tensile strain remains elusive due to the absence of high-resolution in situ correlation techniques. Here, we utilize nanobubble imaging by on-chip total-internal reflection microscopy to visualize active sites on the basal plane of strained MoS2 during hydrogen evolution reaction and atomic force microscopy to correlatively capture the nanoscale morphology and strain maps. By integrating the activity, morphology, and strain maps into comprehensive statistical analyses, we elucidate the strain effect on local activity at both multiprotrusion and (sub)single-protrusion levels. Our findings demonstrate that strain effectively activates sulfur vacancies on the basal plane, with tensile strain significantly enhancing local activity compared to compressive strain. Furthermore, we observe a time-dependent propagation of activity from high-activity to low-activity regions within single protrusions. This work clarifies the interplay between structural morphology and catalytic activity and provides new guidelines for the rational design of optimal TMD catalysts.
- C1[Guo, Shasha] Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY 14853 USA.
[Zhou, Xiuxian; Liu, Xiao; Wu, Yao; Ma, Mingyu; Liu, Zheng] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore.
[Lee, Jinn-kye; Ma, Mingyu; Zhang, Zhengyang] Nanyang Technol Univ, Sch Chem Chem Engn & Biotechnol, Singapore 637371, Singapore.
[Guo, Qing] ASTAR, Inst High Performance Comp IHPC, Singapore 138632, Singapore.
[Guo, Qing] ASTAR, Ctr Frontier AI Res CFAR, Singapore 138632, Singapore.
[Liu, Zheng] Nanyang Technol Univ, CNRS, CINTRA, THALES,UMI 3288, Res Techno Plaza, Singapore 639798, Singapore - C3Cornell University; Nanyang Technological University; Nanyang Technological University; Agency for Science Technology & Research (A*STAR); A*STAR - Institute of High Performance Computing (IHPC); Agency for Science Technology & Research (A*STAR); Nanyang Technological University
- RPLiu, Z (corresponding author), Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore; Zhang, ZY (corresponding author), Nanyang Technol Univ, Sch Chem Chem Engn & Biotechnol, Singapore 637371, Singapore; Liu, Z (corresponding author), Nanyang Technol Univ, CNRS, CINTRA, THALES,UMI 3288, Res Techno Plaza, Singapore 639798, Singapore
- FUAgency for Science, Technology and Research [AcRF Tier 1 RG60/21, RG1/23]; Ministry of Education, Singapore [EDUNC-33-18-279-V12]; Institute for Functional Intelligent Materials [DTC-RGC-04]; National Research Foundation, Singapore [A2084c0065]; Infocomm Media Development Authority under its Trust Tech Funding Initiative [M21K2c0110]; Singapore Agency for Science, Technology, and Research (A*STAR) AME YIRG grant; MTC IRG grant
- FXZ.L. acknowledges funding from the Ministry of Education, Singapore (MOE-MOET2EP10121-0006), and its Research Centre of Excellence award to the Institute for Functional Intelligent Materials (Project EDUNC-33-18-279-V12). Q.G. thanks the support from the National Research Foundation, Singapore, and Infocomm Media Development Authority under its Trust Tech Funding Initiative (DTC-RGC-04). Z.Z. acknowledges the support from the Ministry of Education, Singapore (AcRF Tier 1 RG60/21, RG1/23), and the Singapore Agency for Science, Technology, and Research (A*STAR) AME YIRG grant (A2084c0065) and MTC IRG grant (M21K2c0110).
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- TC0
- Z90
- U10
- U20
- PUAMER CHEMICAL SOC
- PIWASHINGTON
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN0002-7863
- J9J AM CHEM SOC
- JIJ. Am. Chem. Soc.
- PDNOV 8
- PY2024
- DI10.1021/jacs.4c11190
- PG7
- WCChemistry, Multidisciplinary
- SCChemistry
- GAL6H4G
- UTWOS:001351705600001
- ER
- EF
|
Pramanik, Nikhil; Huang, Sunchao; Duan, Ruihuan; Zhai, Qingwei; Go, Michael; Boothroyd, Chris; Liu, Zheng; Wong, Liang Jie Fundamental scaling laws of water-window X-rays from free-electron-driven van der Waals structures NATURE PHOTONICS, 2024, DOI: 10.1038/s41566-024-01547-3. Abstract | BibTeX | Endnote @article{ISI:001345480500002,
title = {Fundamental scaling laws of water-window X-rays from free-electron-driven van der Waals structures},
author = {Nikhil Pramanik and Sunchao Huang and Ruihuan Duan and Qingwei Zhai and Michael Go and Chris Boothroyd and Zheng Liu and Liang Jie Wong},
doi = {10.1038/s41566-024-01547-3},
times_cited = {0},
issn = {1749-4885},
year = {2024},
date = {2024-10-28},
journal = {NATURE PHOTONICS},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {Water-window X-rays are crucial in medical and biological applications, enabling the natural-contrast imaging of biological cells without external staining. However, water-window X-ray sources with bespoke photon energies-needed in high-contrast imaging-remain challenging to obtain, except at large synchrotron facilities. Here we address this challenge by demonstrating tabletop, water-window X-ray generation from free-electron-driven van der Waals materials, enabling the continuous tuning of photon energies across the entire water-window regime. Additionally, we present a truly predictive theoretical framework combining first-principles electromagnetism with Monte Carlo simulations to accurately predict the photon flux and brightness in absolute quantities. We obtain fundamental scaling laws for the tunable photon flux, matching the experimental results and providing a way to design powerful emitters based on free-electron-driven quantum materials. We show that we can potentially achieve photon fluxes needed for imaging and spectroscopy applications (over 10(8) photons s(-1) on the sample-verified by our framework based on our experimentally achieved fluxes of about 10(3) photons s(-1) using similar to 50 nA current). Importantly, our theory highlights the critical role played by the large mean free paths and interlayer atomic spacings unique to van der Waals structures, showing the latter's advantages over other materials in generating water-window X-rays.},
keywords = {},
pubstate = {published},
tppubtype = {article}
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Water-window X-rays are crucial in medical and biological applications, enabling the natural-contrast imaging of biological cells without external staining. However, water-window X-ray sources with bespoke photon energies-needed in high-contrast imaging-remain challenging to obtain, except at large synchrotron facilities. Here we address this challenge by demonstrating tabletop, water-window X-ray generation from free-electron-driven van der Waals materials, enabling the continuous tuning of photon energies across the entire water-window regime. Additionally, we present a truly predictive theoretical framework combining first-principles electromagnetism with Monte Carlo simulations to accurately predict the photon flux and brightness in absolute quantities. We obtain fundamental scaling laws for the tunable photon flux, matching the experimental results and providing a way to design powerful emitters based on free-electron-driven quantum materials. We show that we can potentially achieve photon fluxes needed for imaging and spectroscopy applications (over 10(8) photons s(-1) on the sample-verified by our framework based on our experimentally achieved fluxes of about 10(3) photons s(-1) using similar to 50 nA current). Importantly, our theory highlights the critical role played by the large mean free paths and interlayer atomic spacings unique to van der Waals structures, showing the latter's advantages over other materials in generating water-window X-rays. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUPramanik, N
Huang, SC
Duan, RH
Zhai, QW
Go, M
Boothroyd, C
Liu, Z
Wong, LJ
- AFNikhil Pramanik
Sunchao Huang
Ruihuan Duan
Qingwei Zhai
Michael Go
Chris Boothroyd
Zheng Liu
Liang Jie Wong
- TIFundamental scaling laws of water-window X-rays from free-electron-driven van der Waals structures
- SONATURE PHOTONICS
- LAEnglish
- DTArticle
- IDNONRELATIVISTIC ELECTRONS; COHERENT BREMSSTRAHLUNG; RELATIVISTIC ELECTRONS; FOIL THICKNESS; RADIATION; GRAPHENE; LASER; DISTRIBUTIONS; SPECTROSCOPY; MICROSCOPE
- ABWater-window X-rays are crucial in medical and biological applications, enabling the natural-contrast imaging of biological cells without external staining. However, water-window X-ray sources with bespoke photon energies-needed in high-contrast imaging-remain challenging to obtain, except at large synchrotron facilities. Here we address this challenge by demonstrating tabletop, water-window X-ray generation from free-electron-driven van der Waals materials, enabling the continuous tuning of photon energies across the entire water-window regime. Additionally, we present a truly predictive theoretical framework combining first-principles electromagnetism with Monte Carlo simulations to accurately predict the photon flux and brightness in absolute quantities. We obtain fundamental scaling laws for the tunable photon flux, matching the experimental results and providing a way to design powerful emitters based on free-electron-driven quantum materials. We show that we can potentially achieve photon fluxes needed for imaging and spectroscopy applications (over 10(8) photons s(-1) on the sample-verified by our framework based on our experimentally achieved fluxes of about 10(3) photons s(-1) using similar to 50 nA current). Importantly, our theory highlights the critical role played by the large mean free paths and interlayer atomic spacings unique to van der Waals structures, showing the latter's advantages over other materials in generating water-window X-rays.
- C1[Pramanik, Nikhil; Huang, Sunchao; Zhai, Qingwei; Go, Michael; Wong, Liang Jie] Nanyang Technol Univ, Sch Elect & Elect Engn, Singapore, Singapore.
[Duan, Ruihuan] Nanyang Technol Univ, CINTRA CNRS, NTU, THALES, Singapore, Singapore.
[Duan, Ruihuan; Boothroyd, Chris; Liu, Zheng] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore, Singapore.
[Boothroyd, Chris] Nanyang Technol Univ, Facil Anal Characterisat Testing & Simulat FACTS, Singapore, Singapore.
[Liu, Zheng] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore - C3Nanyang Technological University; Nanyang Technological University; Nanyang Technological University; Nanyang Technological University; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM)
- RPWong, LJ (corresponding author), Nanyang Technol Univ, Sch Elect & Elect Engn, Singapore, Singapore
- FUMinistry of Education - Singapore (MOE) [MOE-T2EP50222-0012]; Ministry of Education, Singapore, under its AcRF Tier 2 programme [MOE-MOET32023-0003]; A*STAR SERC MTC Programmatic Fund; Singapore Ministry of Education Tier 3 Programmatic Fund
- FXWe thank A. Lim, Y. Y. Tay, S. Morris and D. Ang for helpful discussions. This project is supported by the Ministry of Education, Singapore, under its AcRF Tier 2 programme (award no. MOE-T2EP50222-0012). We acknowledge the Facility for Analysis, Characterisation, Testing and Simulation, Nanyang Technological University, Singapore, for use of their electron microscopy/X-ray facilities. Z.L. and R.D. acknowledge the support of A*STAR SERC MTC Programmatic Fund (award no. M23M2b0056) and the Singapore Ministry of Education Tier 3 Programmatic Fund (award no. MOE-MOET32023-0003).
- NR105
- TC0
- Z90
- U10
- U20
- PUNATURE PORTFOLIO
- PIBERLIN
- PAHEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY
- SN1749-4885
- J9NAT PHOTONICS
- JINat. Photonics
- PDOCT 28
- PY2024
- DI10.1038/s41566-024-01547-3
- PG10
- WCOptics; Physics, Applied
- SCOptics; Physics
- GAK7E9B
- UTWOS:001345480500002
- ER
- EF
|
Yi, Kongyang; Wu, Yao; An, Liheng; Deng, Ya; Duan, Ruihuan; Yang, Jiefu; Zhu, Chao; Gao, Weibo; Liu, Zheng Van der Waals Encapsulation by Ultrathin Oxide for Air-Sensitive 2D Materials ADVANCED MATERIALS, 36 (33), 2024, DOI: 10.1002/adma.202403494. Abstract | BibTeX | Endnote @article{ISI:001251534500001,
title = {Van der Waals Encapsulation by Ultrathin Oxide for Air-Sensitive 2D Materials},
author = {Kongyang Yi and Yao Wu and Liheng An and Ya Deng and Ruihuan Duan and Jiefu Yang and Chao Zhu and Weibo Gao and Zheng Liu},
doi = {10.1002/adma.202403494},
times_cited = {0},
issn = {0935-9648},
year = {2024},
date = {2024-06-22},
journal = {ADVANCED MATERIALS},
volume = {36},
number = {33},
publisher = {WILEY-V C H VERLAG GMBH},
address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY},
abstract = {The ambient stability is one of the focal points for applications of 2D materials, especially for those well-known air-sensitive ones, such as black phosphorus (BP) and transitional metal telluride. Traditional methods of encapsulation, such as atomic layer deposition of oxides and heterogeneous integration of hexagonal boron nitride, can hardly avoid removal of encapsulation layer when the 2D materials are encapsulated for further device fabrication, which causes complexity and damage during the procedure. Here, a van der Waals encapsulation method that allows direct device fabrication without removal of encapsulation layer is introduced using Ga2O3 from liquid gallium. Taking advantage of the robust isolation ability against ambient environment of the dense native oxide of gallium, hundreds of times longer retention time of (opto)electronic properties of encapsulated BP and MoTe2 devices is realized than unencapsulated devices. Due to the ultrathin high-kappa properties of Ga2O3, top-gated devices are directly fabricated with the encapsulation layer, simultaneously as a dielectric layer. This direct device fabrication is realized by selective etching of Ga2O3, leaving the encapsulated materials intact. Encapsulated 1T' MoTe2 exhibits high conductivity even after 150 days in ambient environment. This method is, therefore, highlighted as a promising and distinctive one compared with traditional passivation approaches.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The ambient stability is one of the focal points for applications of 2D materials, especially for those well-known air-sensitive ones, such as black phosphorus (BP) and transitional metal telluride. Traditional methods of encapsulation, such as atomic layer deposition of oxides and heterogeneous integration of hexagonal boron nitride, can hardly avoid removal of encapsulation layer when the 2D materials are encapsulated for further device fabrication, which causes complexity and damage during the procedure. Here, a van der Waals encapsulation method that allows direct device fabrication without removal of encapsulation layer is introduced using Ga2O3 from liquid gallium. Taking advantage of the robust isolation ability against ambient environment of the dense native oxide of gallium, hundreds of times longer retention time of (opto)electronic properties of encapsulated BP and MoTe2 devices is realized than unencapsulated devices. Due to the ultrathin high-kappa properties of Ga2O3, top-gated devices are directly fabricated with the encapsulation layer, simultaneously as a dielectric layer. This direct device fabrication is realized by selective etching of Ga2O3, leaving the encapsulated materials intact. Encapsulated 1T' MoTe2 exhibits high conductivity even after 150 days in ambient environment. This method is, therefore, highlighted as a promising and distinctive one compared with traditional passivation approaches. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUYi, KY
Wu, Y
An, LH
Deng, Y
Duan, RH
Yang, JF
Zhu, C
Gao, WB
Liu, Z
- AFKongyang Yi
Yao Wu
Liheng An
Ya Deng
Ruihuan Duan
Jiefu Yang
Chao Zhu
Weibo Gao
Zheng Liu
- TIVan der Waals Encapsulation by Ultrathin Oxide for Air-Sensitive 2D Materials
- SOADVANCED MATERIALS
- LAEnglish
- DTArticle
- DE2D Materials; Ambient Stability; Encapsulation; Field-effect Transistors; Liquid Metal
- IDEXFOLIATED BLACK PHOSPHORUS; EFFECTIVE PASSIVATION; DEGRADATION; SCALE; FILMS
- ABThe ambient stability is one of the focal points for applications of 2D materials, especially for those well-known air-sensitive ones, such as black phosphorus (BP) and transitional metal telluride. Traditional methods of encapsulation, such as atomic layer deposition of oxides and heterogeneous integration of hexagonal boron nitride, can hardly avoid removal of encapsulation layer when the 2D materials are encapsulated for further device fabrication, which causes complexity and damage during the procedure. Here, a van der Waals encapsulation method that allows direct device fabrication without removal of encapsulation layer is introduced using Ga2O3 from liquid gallium. Taking advantage of the robust isolation ability against ambient environment of the dense native oxide of gallium, hundreds of times longer retention time of (opto)electronic properties of encapsulated BP and MoTe2 devices is realized than unencapsulated devices. Due to the ultrathin high-kappa properties of Ga2O3, top-gated devices are directly fabricated with the encapsulation layer, simultaneously as a dielectric layer. This direct device fabrication is realized by selective etching of Ga2O3, leaving the encapsulated materials intact. Encapsulated 1T' MoTe2 exhibits high conductivity even after 150 days in ambient environment. This method is, therefore, highlighted as a promising and distinctive one compared with traditional passivation approaches.
- C1[Yi, Kongyang; Wu, Yao; Deng, Ya; Duan, Ruihuan; Yang, Jiefu; Zhu, Chao; Liu, Zheng] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore.
[An, Liheng; Gao, Weibo] Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore - C3Nanyang Technological University; Nanyang Technological University
- RPLiu, Z (corresponding author), Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore
- FUNational Research Foundation, Singapore, under its Competitive Research Programme (CRP) [NRF-CRP22-2019-0007, NRF-CRP22-2019-0004, NRF2020-NRF-ISF004-3520]; Ministry of Education, Singapore, under its Research Centre of Excellence [EDUNC-33-18-279-V12]; A*STAR under its AME IRG Grant [A2083c0052]; MTC Programmatic Grant [M23M2b0056]
- FXZ.L. acknowledges the support from National Research Foundation, Singapore, under its Competitive Research Programme (CRP) (NRF-CRP22-2019-0007 and NRF-CRP22-2019-0004), under its NRF-ISF joint research program (NRF2020-NRF-ISF004-3520). This research is supported by the Ministry of Education, Singapore, under its Research Centre of Excellence award to the Institute for Functional Intelligent Materials (Project No. EDUNC-33-18-279-V12). This research is also supported by A*STAR under its AME IRG Grant (Project No. A2083c0052) and MTC Programmatic Grant (M23M2b0056).
- NR34
- TC0
- Z90
- U143
- U243
- PUWILEY-V C H VERLAG GMBH
- PIWEINHEIM
- PAPOSTFACH 101161, 69451 WEINHEIM, GERMANY
- SN0935-9648
- J9ADVAN MATER
- JIAdv. Mater.
- PDAUG
- PY2024
- VL36
- DI10.1002/adma.202403494
- PG9
- WCChemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter
- SCChemistry; Science & Technology - Other Topics; Materials Science; Physics
- GAC9T2Z
- UTWOS:001251534500001
- ER
- EF
|
Guo, Huazhang; Lu, Yuhao; Lei, Zhendong; Bao, Hong; Zhang, Mingwan; Wang, Zeming; Guan, Cuntai; Tang, Bijun; Liu, Zheng; Wang, Liang Machine learning-guided realization of full-color high-quantum-yield carbon quantum dots NATURE COMMUNICATIONS, 15 (1), 2024, DOI: 10.1038/s41467-024-49172-6. Abstract | BibTeX | Endnote @article{ISI:001240998200035,
title = {Machine learning-guided realization of full-color high-quantum-yield carbon quantum dots},
author = {Huazhang Guo and Yuhao Lu and Zhendong Lei and Hong Bao and Mingwan Zhang and Zeming Wang and Cuntai Guan and Bijun Tang and Zheng Liu and Liang Wang},
doi = {10.1038/s41467-024-49172-6},
times_cited = {7},
year = {2024},
date = {2024-06-06},
journal = {NATURE COMMUNICATIONS},
volume = {15},
number = {1},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {Carbon quantum dots (CQDs) have versatile applications in luminescence, whereas identifying optimal synthesis conditions has been challenging due to numerous synthesis parameters and multiple desired outcomes, creating an enormous search space. In this study, we present a novel multi-objective optimization strategy utilizing a machine learning (ML) algorithm to intelligently guide the hydrothermal synthesis of CQDs. Our closed-loop approach learns from limited and sparse data, greatly reducing the research cycle and surpassing traditional trial-and-error methods. Moreover, it also reveals the intricate links between synthesis parameters and target properties and unifies the objective function to optimize multiple desired properties like full-color photoluminescence (PL) wavelength and high PL quantum yields (PLQY). With only 63 experiments, we achieve the synthesis of full-color fluorescent CQDs with high PLQY exceeding 60% across all colors. Our study represents a significant advancement in ML-guided CQDs synthesis, setting the stage for developing new materials with multiple desired properties.},
keywords = {},
pubstate = {published},
tppubtype = {article}
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Carbon quantum dots (CQDs) have versatile applications in luminescence, whereas identifying optimal synthesis conditions has been challenging due to numerous synthesis parameters and multiple desired outcomes, creating an enormous search space. In this study, we present a novel multi-objective optimization strategy utilizing a machine learning (ML) algorithm to intelligently guide the hydrothermal synthesis of CQDs. Our closed-loop approach learns from limited and sparse data, greatly reducing the research cycle and surpassing traditional trial-and-error methods. Moreover, it also reveals the intricate links between synthesis parameters and target properties and unifies the objective function to optimize multiple desired properties like full-color photoluminescence (PL) wavelength and high PL quantum yields (PLQY). With only 63 experiments, we achieve the synthesis of full-color fluorescent CQDs with high PLQY exceeding 60% across all colors. Our study represents a significant advancement in ML-guided CQDs synthesis, setting the stage for developing new materials with multiple desired properties. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUGuo, HZ
Lu, YH
Lei, ZD
Bao, H
Zhang, MW
Wang, ZM
Guan, CT
Tang, BJ
Liu, Z
Wang, L
- AFHuazhang Guo
Yuhao Lu
Zhendong Lei
Hong Bao
Mingwan Zhang
Zeming Wang
Cuntai Guan
Bijun Tang
Zheng Liu
Liang Wang
- TIMachine learning-guided realization of full-color high-quantum-yield carbon quantum dots
- SONATURE COMMUNICATIONS
- LAEnglish
- DTArticle
- ABCarbon quantum dots (CQDs) have versatile applications in luminescence, whereas identifying optimal synthesis conditions has been challenging due to numerous synthesis parameters and multiple desired outcomes, creating an enormous search space. In this study, we present a novel multi-objective optimization strategy utilizing a machine learning (ML) algorithm to intelligently guide the hydrothermal synthesis of CQDs. Our closed-loop approach learns from limited and sparse data, greatly reducing the research cycle and surpassing traditional trial-and-error methods. Moreover, it also reveals the intricate links between synthesis parameters and target properties and unifies the objective function to optimize multiple desired properties like full-color photoluminescence (PL) wavelength and high PL quantum yields (PLQY). With only 63 experiments, we achieve the synthesis of full-color fluorescent CQDs with high PLQY exceeding 60% across all colors. Our study represents a significant advancement in ML-guided CQDs synthesis, setting the stage for developing new materials with multiple desired properties.
- C1[Guo, Huazhang; Bao, Hong; Zhang, Mingwan; Wang, Zeming; Wang, Liang] Shanghai Univ, Inst Nanochem & Nanobiol, Sch Environm & Chem Engn, 99 Shangda Rd, Shanghai 200444, Peoples R China.
[Lu, Yuhao; Guan, Cuntai] Nanyang Technol Univ, Coll Comp & Data Sci, 50 Nanyang Ave, Singapore 639798, Singapore.
[Lei, Zhendong; Tang, Bijun; Liu, Zheng; Wang, Liang] Nanyang Technol Univ, Sch Mat Sci & Engn, 50 Nanyang Ave, Singapore 639798, Singapore.
[Liu, Zheng] CINTRA CNRS NTU THALES, UMI 3288, Res Techno Plaza,50 Nanyang Dr,Border 10 Block,Lev, Singapore 637553, Singapore.
[Liu, Zheng] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore - C3Shanghai University; Nanyang Technological University; Nanyang Technological University; Nanyang Technological University; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM)
- RPWang, L (corresponding author), Shanghai Univ, Inst Nanochem & Nanobiol, Sch Environm & Chem Engn, 99 Shangda Rd, Shanghai 200444, Peoples R China; Guan, CT (corresponding author), Nanyang Technol Univ, Coll Comp & Data Sci, 50 Nanyang Ave, Singapore 639798, Singapore; Tang, BJ (corresponding author), Nanyang Technol Univ, Sch Mat Sci & Engn, 50 Nanyang Ave, Singapore 639798, Singapore; Liu, Z (corresponding author), CINTRA CNRS NTU THALES, UMI 3288, Res Techno Plaza,50 Nanyang Dr,Border 10 Block,Lev, Singapore 637553, Singapore; Liu, Z (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore
- FUMinistry of Education - Singapore (MOE) [21PJD022]; Shanghai Pujiang Program [2023T160406]; China Postdoctoral Science Foundation [21901154]; National Natural Science Foundation of China [EDUNC-33-18-279-V12]; Ministry of Education, Singapore, under its Research Centre of Excellence award [AISG2-GC-2023-009]; Institute for Functional Intelligent Materials; National Research Foundation, Singapore, under its AI Singapore Programme; Presidential Postdoctoral Fellowship of Nanyang Technological University
- FXThis project was funded by the Shanghai Pujiang Program (Project No. 21PJD022 to L.W.), China Postdoctoral Science Foundation (Project No. 2023T160406 to H.G.), and the National Natural Science Foundation of China (Project No. 21901154 to L.W.). This project was also supported by the Ministry of Education, Singapore, under its Research Centre of Excellence award to the Institute for Functional Intelligent Materials (Project No. EDUNC-33-18-279-V12 to Z.L.), National Research Foundation, Singapore, under its AI Singapore Programme (AISG Award No: AISG2-GC-2023-009 to Z.L., B.T., and C.G.), as well as the Presidential Postdoctoral Fellowship of Nanyang Technological University (B.T.).
- NR62
- TC7
- Z97
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Guo, Shasha; Ma, Mingyu; Wang, Yuqing; Wang, Jinbo; Jiang, Yubin; Duan, Ruihuan; Lei, Zhendong; Wang, Shuangyin; He, Yongmin; Liu, Zheng Spatially Confined Microcells: A Path toward TMD Catalyst Design CHEMICAL REVIEWS, 124 (11), pp. 6952-7006, 2024, DOI: 10.1021/acs.chemrev.3c00711. Abstract | BibTeX | Endnote @article{ISI:001226137500001,
title = {Spatially Confined Microcells: A Path toward TMD Catalyst Design},
author = {Shasha Guo and Mingyu Ma and Yuqing Wang and Jinbo Wang and Yubin Jiang and Ruihuan Duan and Zhendong Lei and Shuangyin Wang and Yongmin He and Zheng Liu},
doi = {10.1021/acs.chemrev.3c00711},
times_cited = {1},
issn = {0009-2665},
year = {2024},
date = {2024-05-15},
journal = {CHEMICAL REVIEWS},
volume = {124},
number = {11},
pages = {6952-7006},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {With the ability to maximize the exposure of nearly all active sites to reactions, two-dimensional transition metal dichalcogenide (TMD) has become a fascinating new class of materials for electrocatalysis. Recently, electrochemical microcells have been developed, and their unique spatial-confined capability enables understanding of catalytic behaviors at a single material level, significantly promoting this field. This Review provides an overview of the recent progress in microcell-based TMD electrocatalyst studies. We first introduced the structural characteristics of TMD materials and discussed their site engineering strategies for electrocatalysis. Later, we comprehensively described two distinct types of microcells: the window-confined on-chip electrochemical microcell (OCEM) and the droplet-confined scanning electrochemical cell microscopy (SECCM). Their setups, working principles, and instrumentation were elucidated in detail, respectively. Furthermore, we summarized recent advances of OCEM and SECCM obtained in TMD catalysts, such as active site identification and imaging, site monitoring, modulation of charge injection and transport, and electrostatic field gating. Finally, we discussed the current challenges and provided personal perspectives on electrochemical microcell research.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
With the ability to maximize the exposure of nearly all active sites to reactions, two-dimensional transition metal dichalcogenide (TMD) has become a fascinating new class of materials for electrocatalysis. Recently, electrochemical microcells have been developed, and their unique spatial-confined capability enables understanding of catalytic behaviors at a single material level, significantly promoting this field. This Review provides an overview of the recent progress in microcell-based TMD electrocatalyst studies. We first introduced the structural characteristics of TMD materials and discussed their site engineering strategies for electrocatalysis. Later, we comprehensively described two distinct types of microcells: the window-confined on-chip electrochemical microcell (OCEM) and the droplet-confined scanning electrochemical cell microscopy (SECCM). Their setups, working principles, and instrumentation were elucidated in detail, respectively. Furthermore, we summarized recent advances of OCEM and SECCM obtained in TMD catalysts, such as active site identification and imaging, site monitoring, modulation of charge injection and transport, and electrostatic field gating. Finally, we discussed the current challenges and provided personal perspectives on electrochemical microcell research. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUGuo, SS
Ma, MY
Wang, YQ
Wang, JB
Jiang, YB
Duan, RH
Lei, ZD
Wang, SY
He, YM
Liu, Z
- AFShasha Guo
Mingyu Ma
Yuqing Wang
Jinbo Wang
Yubin Jiang
Ruihuan Duan
Zhendong Lei
Shuangyin Wang
Yongmin He
Zheng Liu
- TISpatially Confined Microcells: A Path toward TMD Catalyst Design
- SOCHEMICAL REVIEWS
- LAEnglish
- DTArticle
- IDTRANSITION-METAL DICHALCOGENIDE; ELECTROCHEMICAL-CELL MICROSCOPY; HYDROGEN EVOLUTION REACTION; CHIP ELECTROCATALYTIC MICRODEVICE; INDUCED PHASE-TRANSITION; WAFER-SCALE; GRAIN-BOUNDARIES; MOS2 NANOSHEETS; ACTIVE-SITES; BASAL PLANES
- ABWith the ability to maximize the exposure of nearly all active sites to reactions, two-dimensional transition metal dichalcogenide (TMD) has become a fascinating new class of materials for electrocatalysis. Recently, electrochemical microcells have been developed, and their unique spatial-confined capability enables understanding of catalytic behaviors at a single material level, significantly promoting this field. This Review provides an overview of the recent progress in microcell-based TMD electrocatalyst studies. We first introduced the structural characteristics of TMD materials and discussed their site engineering strategies for electrocatalysis. Later, we comprehensively described two distinct types of microcells: the window-confined on-chip electrochemical microcell (OCEM) and the droplet-confined scanning electrochemical cell microscopy (SECCM). Their setups, working principles, and instrumentation were elucidated in detail, respectively. Furthermore, we summarized recent advances of OCEM and SECCM obtained in TMD catalysts, such as active site identification and imaging, site monitoring, modulation of charge injection and transport, and electrostatic field gating. Finally, we discussed the current challenges and provided personal perspectives on electrochemical microcell research.
- C1[Guo, Shasha; Ma, Mingyu; Wang, Yuqing; Duan, Ruihuan; Lei, Zhendong; Liu, Zheng] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore.
[Guo, Shasha] Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY 14853 USA.
[Ma, Mingyu] Nanyang Technol Univ, Sch Chem Chem Engn & Biotechnol, Singapore 637616, Singapore.
[Wang, Jinbo; Jiang, Yubin; Wang, Shuangyin; He, Yongmin] Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chemobiosensing & Chemometr, Changsha 410082, Peoples R China.
[Duan, Ruihuan; Liu, Zheng] CINTRA CNRS NTU THALES, UMI 3288, Singapore 639798, Singapore.
[Liu, Zheng] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore - C3Nanyang Technological University; Cornell University; Nanyang Technological University; Hunan University; Nanyang Technological University; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore
- RPLiu, Z (corresponding author), Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore; He, YM (corresponding author), Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chemobiosensing & Chemometr, Changsha 410082, Peoples R China; Liu, Z (corresponding author), CINTRA CNRS NTU THALES, UMI 3288, Singapore 639798, Singapore; Liu, Z (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore
- FUMinistry of Education - Singapore [AcRF MOE2019-T2-2-105, AcRF Tier 1 RG7/21]; Singapore Ministry of Education [2021YFA1500900]; National Key R&D Program of China [531119200209]; Fundamental Research Funds for Central Universities [52203354, 22272048]; National Natural Science Foundation of China
- FXZ.L. acknowledges funding from the Singapore Ministry of Education (AcRF MOE2019-T2-2-105 and AcRF Tier 1 RG7/21). Y.H. acknowledges the National Key R&D Program of China (2021YFA1500900), the Fundamental Research Funds for Central Universities (531119200209), and the National Natural Science Foundation of China (52203354 and 22272048).
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