2025
|
Chen, Jinxing; Li, Jiali; Hai, Xiao; Li, Jun; Zhang, Tao; Lu, Jiong The Prospect of Single-Atom Catalysis Empowered by Designer Dynamics and
Machine Intelligence JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 147 (49), pp. 44617-44632, 2025, DOI: 10.1021/jacs.5c13920. Abstract | BibTeX | Endnote @article{WOS:001623147900001,
title = {The Prospect of Single-Atom Catalysis Empowered by Designer Dynamics and
Machine Intelligence},
author = {Jinxing Chen and Jiali Li and Xiao Hai and Jun Li and Tao Zhang and Jiong Lu},
doi = {10.1021/jacs.5c13920},
times_cited = {2},
issn = {0002-7863},
year = {2025},
date = {2025-12-01},
journal = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY},
volume = {147},
number = {49},
pages = {44617-44632},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Heterogeneous single-atom catalysts (SACs) represent a vibrant frontier
in catalysis science and technology and are characterized by
well-defined, atomically precise catalytic active centers and maximized
metal atom utilization, enabling chemical transformation with
exceptional activity and selectivity. The local coordination
environments of SACs can be precisely tailored by surrounding atoms,
akin to homogeneous catalysts where metal atoms are coordinated by
organic ligands. Unlike adaptive ligands in homogeneous catalysts,
heterogeneous SACs immobilized on stable and rigid supports are
typically less dynamic even under relatively harsh reaction conditions.
This can enhance the stability of the catalyst but constrain their
catalytic capabilities and limit their reaction scope. However, with the
rapid advancement of in situ and operando characterization tools, the
reversible evolution of structural and electronic properties at active
sites during reactions has been revealed in SACs, which exhibit
extraordinary dynamic behaviors. These SACs feature unique local
coordination environments that enable highly adaptive behaviors,
enhancing their activity and selectivity while maintaining stability and
preventing metal leaching during reactions. This perspective highlights
recent progress in the development of such adaptive SACs and provides
molecular-level insights into their adaptive and reversible structural
changes during reactions. It offers a comprehensive overview of the
transformative implications of SACs' dynamics and illustrates how these
properties can be modeled and harnessed. Finally, we discuss the
challenges and opportunities in designing adaptive SACs by leveraging
molecular-level insights and machine intelligence with high-throughput
automation platforms to drive industrially crucial sustainable chemical
transformations.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Heterogeneous single-atom catalysts (SACs) represent a vibrant frontier
in catalysis science and technology and are characterized by
well-defined, atomically precise catalytic active centers and maximized
metal atom utilization, enabling chemical transformation with
exceptional activity and selectivity. The local coordination
environments of SACs can be precisely tailored by surrounding atoms,
akin to homogeneous catalysts where metal atoms are coordinated by
organic ligands. Unlike adaptive ligands in homogeneous catalysts,
heterogeneous SACs immobilized on stable and rigid supports are
typically less dynamic even under relatively harsh reaction conditions.
This can enhance the stability of the catalyst but constrain their
catalytic capabilities and limit their reaction scope. However, with the
rapid advancement of in situ and operando characterization tools, the
reversible evolution of structural and electronic properties at active
sites during reactions has been revealed in SACs, which exhibit
extraordinary dynamic behaviors. These SACs feature unique local
coordination environments that enable highly adaptive behaviors,
enhancing their activity and selectivity while maintaining stability and
preventing metal leaching during reactions. This perspective highlights
recent progress in the development of such adaptive SACs and provides
molecular-level insights into their adaptive and reversible structural
changes during reactions. It offers a comprehensive overview of the
transformative implications of SACs' dynamics and illustrates how these
properties can be modeled and harnessed. Finally, we discuss the
challenges and opportunities in designing adaptive SACs by leveraging
molecular-level insights and machine intelligence with high-throughput
automation platforms to drive industrially crucial sustainable chemical
transformations. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFJinxing Chen
Jiali Li
Xiao Hai
Jun Li
Tao Zhang
Jiong Lu
- TIThe Prospect of Single-Atom Catalysis Empowered by Designer Dynamics and
Machine Intelligence - SOJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
- DTArticle
- ABHeterogeneous single-atom catalysts (SACs) represent a vibrant frontier
in catalysis science and technology and are characterized by
well-defined, atomically precise catalytic active centers and maximized
metal atom utilization, enabling chemical transformation with
exceptional activity and selectivity. The local coordination
environments of SACs can be precisely tailored by surrounding atoms,
akin to homogeneous catalysts where metal atoms are coordinated by
organic ligands. Unlike adaptive ligands in homogeneous catalysts,
heterogeneous SACs immobilized on stable and rigid supports are
typically less dynamic even under relatively harsh reaction conditions.
This can enhance the stability of the catalyst but constrain their
catalytic capabilities and limit their reaction scope. However, with the
rapid advancement of in situ and operando characterization tools, the
reversible evolution of structural and electronic properties at active
sites during reactions has been revealed in SACs, which exhibit
extraordinary dynamic behaviors. These SACs feature unique local
coordination environments that enable highly adaptive behaviors,
enhancing their activity and selectivity while maintaining stability and
preventing metal leaching during reactions. This perspective highlights
recent progress in the development of such adaptive SACs and provides
molecular-level insights into their adaptive and reversible structural
changes during reactions. It offers a comprehensive overview of the
transformative implications of SACs' dynamics and illustrates how these
properties can be modeled and harnessed. Finally, we discuss the
challenges and opportunities in designing adaptive SACs by leveraging
molecular-level insights and machine intelligence with high-throughput
automation platforms to drive industrially crucial sustainable chemical
transformations. - Z92
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN0002-7863
- VL147
- BP44617
- EP44632
- DI10.1021/jacs.5c13920
- UTWOS:001623147900001
- ER
- EF
|
Zhang, Zhi; Zhang, Yuwei; Lu, Kangjun; Zhang, Jun-Jie; Zhang, Nannan; Feng, Rui; Ye, Haoran; Zhou, Xiaoli; Li, Linglong; Wan, Dongyang; Lu, Junpeng; Ni, Zhenhua; Wang, Jinlan; Chen, Qian; Lu, Jiong; Li, Zejun Near-100% spontaneous rolling up of polar van der Waals materials NATURE MATERIALS, 24 (11), 2025, DOI: 10.1038/s41563-025-02357-w. Abstract | BibTeX | Endnote @article{WOS:001592760400001,
title = {Near-100% spontaneous rolling up of polar van der Waals materials},
author = {Zhi Zhang and Yuwei Zhang and Kangjun Lu and Jun-Jie Zhang and Nannan Zhang and Rui Feng and Haoran Ye and Xiaoli Zhou and Linglong Li and Dongyang Wan and Junpeng Lu and Zhenhua Ni and Jinlan Wang and Qian Chen and Jiong Lu and Zejun Li},
doi = {10.1038/s41563-025-02357-w},
times_cited = {2},
issn = {1476-1122},
year = {2025},
date = {2025-11-01},
journal = {NATURE MATERIALS},
volume = {24},
number = {11},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {Rolling two-dimensional materials into one-dimensional nanoscrolls
introduces curvature, chirality and symmetry breaking, enabling emergent
properties. Conventional methods relying on external driving forces,
however, exhibit poor control, low yield and limited reproducibility.
Here we report spontaneous scrolling in polar van der Waals materials
via an electrochemical intercalation/exfoliation process, enabling
scalable nanoscroll production. This self-rolling is driven
intrinsically by out-of-plane electric polarization (P-perpendicular
to), where the magnitude of P-perpendicular to is modulated by the
intercalant size. Validated across eight polar materials, this approach
achieves virtually 100% yield and reproducibility with defined
scrolling direction, surpassing external driving force limitations. The
nanoscrolls exhibit layer-independent inversion symmetry breaking and
coherently enhanced second-harmonic generation, exceeding
two-dimensional flakes by similar to 100-fold and rivalling leading
two-dimensional nonlinear materials. Electrochemical initiation further
facilitates metal-ion co-intercalation, yielding ten hybrid nanoscroll
architectures. These findings establish a scalable route to create
one-dimensional nanostructures and hybrid heterostructures, paving the
way for designer quantum solids and van der Waals superlattices in
quantum nanodevices.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Rolling two-dimensional materials into one-dimensional nanoscrolls
introduces curvature, chirality and symmetry breaking, enabling emergent
properties. Conventional methods relying on external driving forces,
however, exhibit poor control, low yield and limited reproducibility.
Here we report spontaneous scrolling in polar van der Waals materials
via an electrochemical intercalation/exfoliation process, enabling
scalable nanoscroll production. This self-rolling is driven
intrinsically by out-of-plane electric polarization (P-perpendicular
to), where the magnitude of P-perpendicular to is modulated by the
intercalant size. Validated across eight polar materials, this approach
achieves virtually 100% yield and reproducibility with defined
scrolling direction, surpassing external driving force limitations. The
nanoscrolls exhibit layer-independent inversion symmetry breaking and
coherently enhanced second-harmonic generation, exceeding
two-dimensional flakes by similar to 100-fold and rivalling leading
two-dimensional nonlinear materials. Electrochemical initiation further
facilitates metal-ion co-intercalation, yielding ten hybrid nanoscroll
architectures. These findings establish a scalable route to create
one-dimensional nanostructures and hybrid heterostructures, paving the
way for designer quantum solids and van der Waals superlattices in
quantum nanodevices. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFZhi Zhang
Yuwei Zhang
Kangjun Lu
Jun-Jie Zhang
Nannan Zhang
Rui Feng
Haoran Ye
Xiaoli Zhou
Linglong Li
Dongyang Wan
Junpeng Lu
Zhenhua Ni
Jinlan Wang
Qian Chen
Jiong Lu
Zejun Li
- TINear-100% spontaneous rolling up of polar van der Waals materials
- SONATURE MATERIALS
- DTArticle
- ABRolling two-dimensional materials into one-dimensional nanoscrolls
introduces curvature, chirality and symmetry breaking, enabling emergent
properties. Conventional methods relying on external driving forces,
however, exhibit poor control, low yield and limited reproducibility.
Here we report spontaneous scrolling in polar van der Waals materials
via an electrochemical intercalation/exfoliation process, enabling
scalable nanoscroll production. This self-rolling is driven
intrinsically by out-of-plane electric polarization (P-perpendicular
to), where the magnitude of P-perpendicular to is modulated by the
intercalant size. Validated across eight polar materials, this approach
achieves virtually 100% yield and reproducibility with defined
scrolling direction, surpassing external driving force limitations. The
nanoscrolls exhibit layer-independent inversion symmetry breaking and
coherently enhanced second-harmonic generation, exceeding
two-dimensional flakes by similar to 100-fold and rivalling leading
two-dimensional nonlinear materials. Electrochemical initiation further
facilitates metal-ion co-intercalation, yielding ten hybrid nanoscroll
architectures. These findings establish a scalable route to create
one-dimensional nanostructures and hybrid heterostructures, paving the
way for designer quantum solids and van der Waals superlattices in
quantum nanodevices. - Z92
- PUNATURE PORTFOLIO
- PAHEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY
- SN1476-1122
- VL24
- DI10.1038/s41563-025-02357-w
- UTWOS:001592760400001
- ER
- EF
|
Song, Shaotang; Lu, Jiong Merging d- and π-electron magnetism: Graphene nanoribbons NATURE CHEMISTRY, 17 (9), pp. 1307-1308, 2025, DOI: 10.1038/s41557-025-01923-8. Abstract | BibTeX | Endnote @article{WOS:001558209300001,
title = {Merging d- and π-electron magnetism: Graphene nanoribbons},
author = {Shaotang Song and Jiong Lu},
doi = {10.1038/s41557-025-01923-8},
times_cited = {0},
issn = {1755-4330},
year = {2025},
date = {2025-09-01},
journal = {NATURE CHEMISTRY},
volume = {17},
number = {9},
pages = {1307-1308},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {The development of materials with tunable electronic and magnetic
properties contributes to the advancement of spintronic technologies and
optoelectronics. Now, the combination of IT-and d-electron magnetism has
been achieved through the lateral fusion of periodic metalloporphyrins
along the zigzag edges of graphene nanoribbons.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The development of materials with tunable electronic and magnetic
properties contributes to the advancement of spintronic technologies and
optoelectronics. Now, the combination of IT-and d-electron magnetism has
been achieved through the lateral fusion of periodic metalloporphyrins
along the zigzag edges of graphene nanoribbons. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFShaotang Song
Jiong Lu
- TIMerging d- and π-electron magnetism: Graphene nanoribbons
- SONATURE CHEMISTRY
- DTArticle
- ABThe development of materials with tunable electronic and magnetic
properties contributes to the advancement of spintronic technologies and
optoelectronics. Now, the combination of IT-and d-electron magnetism has
been achieved through the lateral fusion of periodic metalloporphyrins
along the zigzag edges of graphene nanoribbons. - Z90
- PUNATURE PORTFOLIO
- PAHEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY
- SN1755-4330
- VL17
- BP1307
- EP1308
- DI10.1038/s41557-025-01923-8
- UTWOS:001558209300001
- ER
- EF
|
Peng, Xinnan; Lu, Jiong Spin-1/2 Heisenberg chains realized in π-electron systems NATURE SYNTHESIS, 4 (6), pp. 668-670, 2025, DOI: 10.1038/s44160-025-00757-z. BibTeX | Endnote @article{WOS:001428096000001,
title = {Spin-1/2 Heisenberg chains realized in π-electron systems},
author = {Xinnan Peng and Jiong Lu},
doi = {10.1038/s44160-025-00757-z},
times_cited = {2},
year = {2025},
date = {2025-06-01},
journal = {NATURE SYNTHESIS},
volume = {4},
number = {6},
pages = {668-670},
publisher = {SPRINGERNATURE},
address = {CAMPUS, 4 CRINAN ST, LONDON, N1 9XW, ENGLAND},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
- FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFXinnan Peng
Jiong Lu
- TISpin-1/2 Heisenberg chains realized in π-electron systems
- SONATURE SYNTHESIS
- DTArticle
- Z92
- PUSPRINGERNATURE
- PACAMPUS, 4 CRINAN ST, LONDON, N1 9XW, ENGLAND
- VL4
- BP668
- EP670
- DI10.1038/s44160-025-00757-z
- UTWOS:001428096000001
- ER
- EF
|
Sun, Tao; Yang, Tong; Zang, Wenjie; Li, Jing; Sheng, Xiaoyu; Liu, Enzhou; Li, Jiali; Hai, Xiao; Lin, Huihui; Chuang, Cheng-Hao; Su, Chenliang; Fan, Maohong; Yang, Ming; Lin, Ming; Xi, Shibo; Zou, Ruqiang; Lu, Jiong Atomic Gap-State Engineering of MoS2 for Alkaline Water and
Seawater Splitting 47 ACS NANO, 19 (5), pp. 5447-5459, 2025, DOI: 10.1021/acsnano.4c13736. Abstract | BibTeX | Endnote @article{WOS:001395823800001,
title = {Atomic Gap-State Engineering of MoS2 for Alkaline Water and
Seawater Splitting},
author = {Tao Sun and Tong Yang and Wenjie Zang and Jing Li and Xiaoyu Sheng and Enzhou Liu and Jiali Li and Xiao Hai and Huihui Lin and Cheng-Hao Chuang and Chenliang Su and Maohong Fan and Ming Yang and Ming Lin and Shibo Xi and Ruqiang Zou and Jiong Lu},
doi = {10.1021/acsnano.4c13736},
times_cited = {47},
issn = {1936-0851},
year = {2025},
date = {2025-01-01},
journal = {ACS NANO},
volume = {19},
number = {5},
pages = {5447-5459},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Transition-metal dichalcogenides (TMDs), such as molybdenum disulfide
(MoS2), have emerged as a generation of nonprecious catalysts for the
hydrogen evolution reaction (HER), largely due to their theoretical
hydrogen adsorption energy close to that of platinum. However, efforts
to activate the basal planes of TMDs have primarily centered around
strategies such as introducing numerous atomic vacancies, creating
vacancy-heteroatom complexes, or applying significant strain, especially
for acidic media. These approaches, while potentially effective, present
substantial challenges in practical large-scale deployment. Here, we
report a gap-state engineering strategy for the controlled activation of
S atom in MoS2 basal planes through metal single-atom doping,
effectively tackling both efficiency and stability challenges in
alkaline water and seawater splitting. A versatile synthetic methodology
allows for the fabrication of a series of single-metal atom-doped MoS2
materials (M1/MoS2), featuring widely tunable densities with each dopant
replacing a Mo site. Among these (Mn1, Fe1, Co1, and Ni1), Co1/MoS2
demonstrates outstanding HER performance in both alkaline and seawater
alkaline media, with overpotentials at a mere 159 and 164 mV at 100 mA
cm-2, and Tafel slopes at 41 and 45 mV dec-1, respectively, which
surpasses all reported TMD-based nonprecious materials and benchmark
Pt/C catalysts in HER efficiency and stability during seawater
splitting, which can be attributed to an optimal gap-state modulation
associated with sulfur atoms. Experimental data correlating doping
density and dopant identity with HER performance, in conjunction with
theoretical calculations, also reveal a descriptor linked to near-Fermi
gap state modulation, corroborated by the observed increase in
unoccupied S 3p states.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Transition-metal dichalcogenides (TMDs), such as molybdenum disulfide
(MoS2), have emerged as a generation of nonprecious catalysts for the
hydrogen evolution reaction (HER), largely due to their theoretical
hydrogen adsorption energy close to that of platinum. However, efforts
to activate the basal planes of TMDs have primarily centered around
strategies such as introducing numerous atomic vacancies, creating
vacancy-heteroatom complexes, or applying significant strain, especially
for acidic media. These approaches, while potentially effective, present
substantial challenges in practical large-scale deployment. Here, we
report a gap-state engineering strategy for the controlled activation of
S atom in MoS2 basal planes through metal single-atom doping,
effectively tackling both efficiency and stability challenges in
alkaline water and seawater splitting. A versatile synthetic methodology
allows for the fabrication of a series of single-metal atom-doped MoS2
materials (M1/MoS2), featuring widely tunable densities with each dopant
replacing a Mo site. Among these (Mn1, Fe1, Co1, and Ni1), Co1/MoS2
demonstrates outstanding HER performance in both alkaline and seawater
alkaline media, with overpotentials at a mere 159 and 164 mV at 100 mA
cm-2, and Tafel slopes at 41 and 45 mV dec-1, respectively, which
surpasses all reported TMD-based nonprecious materials and benchmark
Pt/C catalysts in HER efficiency and stability during seawater
splitting, which can be attributed to an optimal gap-state modulation
associated with sulfur atoms. Experimental data correlating doping
density and dopant identity with HER performance, in conjunction with
theoretical calculations, also reveal a descriptor linked to near-Fermi
gap state modulation, corroborated by the observed increase in
unoccupied S 3p states. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFTao Sun
Tong Yang
Wenjie Zang
Jing Li
Xiaoyu Sheng
Enzhou Liu
Jiali Li
Xiao Hai
Huihui Lin
Cheng-Hao Chuang
Chenliang Su
Maohong Fan
Ming Yang
Ming Lin
Shibo Xi
Ruqiang Zou
Jiong Lu
- TIAtomic Gap-State Engineering of MoS2 for Alkaline Water and
Seawater Splitting - SOACS NANO
- DTArticle
- ABTransition-metal dichalcogenides (TMDs), such as molybdenum disulfide
(MoS2), have emerged as a generation of nonprecious catalysts for the
hydrogen evolution reaction (HER), largely due to their theoretical
hydrogen adsorption energy close to that of platinum. However, efforts
to activate the basal planes of TMDs have primarily centered around
strategies such as introducing numerous atomic vacancies, creating
vacancy-heteroatom complexes, or applying significant strain, especially
for acidic media. These approaches, while potentially effective, present
substantial challenges in practical large-scale deployment. Here, we
report a gap-state engineering strategy for the controlled activation of
S atom in MoS2 basal planes through metal single-atom doping,
effectively tackling both efficiency and stability challenges in
alkaline water and seawater splitting. A versatile synthetic methodology
allows for the fabrication of a series of single-metal atom-doped MoS2
materials (M1/MoS2), featuring widely tunable densities with each dopant
replacing a Mo site. Among these (Mn1, Fe1, Co1, and Ni1), Co1/MoS2
demonstrates outstanding HER performance in both alkaline and seawater
alkaline media, with overpotentials at a mere 159 and 164 mV at 100 mA
cm-2, and Tafel slopes at 41 and 45 mV dec-1, respectively, which
surpasses all reported TMD-based nonprecious materials and benchmark
Pt/C catalysts in HER efficiency and stability during seawater
splitting, which can be attributed to an optimal gap-state modulation
associated with sulfur atoms. Experimental data correlating doping
density and dopant identity with HER performance, in conjunction with
theoretical calculations, also reveal a descriptor linked to near-Fermi
gap state modulation, corroborated by the observed increase in
unoccupied S 3p states. - Z947
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN1936-0851
- VL19
- BP5447
- EP5459
- DI10.1021/acsnano.4c13736
- UTWOS:001395823800001
- ER
- EF
|