2025
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Liu, Xiongfang; Yang, Tong; Chen, Shanquan; Wu, Jing; Tang, Chi Sin; Ning, Yuanjie; Chen, Zuhuang; Dai, Liang; Sun, Mengxia; Chen, Mingyao; Han, Kun; Zhou, Difan; Zeng, Shengwei; Sun, Shuo; Li, Sensen; Yang, Ming; Breese, Mark B H; Cai, Chuanbing; Venkatesan, Thirumalai; Wee, Andrew T S; Yin, Xinmao Small polarons mediated near-room-temperature metal-insulator transition in vanadium dioxide and their hopping dynamics Journal Article APPLIED PHYSICS REVIEWS, 12 (1), 2025, ISSN: 1931-9401. Abstract | Links | BibTeX @article{ISI:001403236800001,
title = {Small polarons mediated near-room-temperature metal-insulator transition in vanadium dioxide and their hopping dynamics},
author = {Xiongfang Liu and Tong Yang and Shanquan Chen and Jing Wu and Chi Sin Tang and Yuanjie Ning and Zuhuang Chen and Liang Dai and Mengxia Sun and Mingyao Chen and Kun Han and Difan Zhou and Shengwei Zeng and Shuo Sun and Sensen Li and Ming Yang and Mark B H Breese and Chuanbing Cai and Thirumalai Venkatesan and Andrew T S Wee and Xinmao Yin},
doi = {10.1063/5.0236807},
times_cited = {0},
issn = {1931-9401},
year = {2025},
date = {2025-03-01},
journal = {APPLIED PHYSICS REVIEWS},
volume = {12},
number = {1},
publisher = {AIP Publishing},
address = {1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA},
abstract = {Researchers pursuing advanced photoelectric devices have discovered near room-temperature metal-insulator transitions (MIT) in nonvolatile VO2. Despite theoretical investigations suggesting that polaron dynamics mediate the MIT, direct experimental evidence remains scarce. In this study, we present direct evidence of the polaron state in insulating VO2 through high-resolution spectroscopic ellipsometry measurements and first-principles calculations. We illustrate the complementary role of polaron dynamics in facilitating Peierls and Mott transitions, thereby contributing to the MIT processes. Furthermore, our observations and characterizations of conventional metallic and correlated plasmons in the respective phases of the VO2 film offer valuable insight into their electron structures. This investigation enhances comprehension of the MIT mechanism in correlated systems and underscores the roles of polarons, lattice distortions, and electron correlations in facilitating phase transition processes in strongly correlated systems. Additionally, the detailed detection of small polarons and plasmons serves as inspiration for the development of new device functionalities.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Researchers pursuing advanced photoelectric devices have discovered near room-temperature metal-insulator transitions (MIT) in nonvolatile VO2. Despite theoretical investigations suggesting that polaron dynamics mediate the MIT, direct experimental evidence remains scarce. In this study, we present direct evidence of the polaron state in insulating VO2 through high-resolution spectroscopic ellipsometry measurements and first-principles calculations. We illustrate the complementary role of polaron dynamics in facilitating Peierls and Mott transitions, thereby contributing to the MIT processes. Furthermore, our observations and characterizations of conventional metallic and correlated plasmons in the respective phases of the VO2 film offer valuable insight into their electron structures. This investigation enhances comprehension of the MIT mechanism in correlated systems and underscores the roles of polarons, lattice distortions, and electron correlations in facilitating phase transition processes in strongly correlated systems. Additionally, the detailed detection of small polarons and plasmons serves as inspiration for the development of new device functionalities. |
Jiang, Yingying; Wong, Zicong Marvin; Yan, Hongwei; Tan, Teck Leong; Mirsaidov, Utkur Revealing Multistep Phase Separation in Metal Alloy Nanoparticles with In Situ Transmission Electron Microscopy Journal Article ACS NANO, 19 (3), pp. 3886-3894, 2025, ISSN: 1936-0851. Abstract | Links | BibTeX @article{ISI:001396476700001,
title = {Revealing Multistep Phase Separation in Metal Alloy Nanoparticles with \textit{In Situ} Transmission Electron Microscopy},
author = {Yingying Jiang and Zicong Marvin Wong and Hongwei Yan and Teck Leong Tan and Utkur Mirsaidov},
doi = {10.1021/acsnano.4c16095},
times_cited = {0},
issn = {1936-0851},
year = {2025},
date = {2025-01-14},
journal = {ACS NANO},
volume = {19},
number = {3},
pages = {3886-3894},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Phase separation plays a crucial role in many natural and industrial processes, such as the formation of clouds and minerals and the distillation of crude oil. In metals and alloys, phase separation is an important approach often utilized to improve their mechanical strength for use in construction, automobile, and aerospace manufacturing. Despite its importance in many processes, the atomic details of phase separation are largely unknown. In particular, it is unclear how a different crystal phase emerges from the parent alloy. Here, using real-time in situ transmission electron microscopy, we describe the stages of the phase separation in face-centered cubic (fcc) AuRu alloy nanoparticles, resulting in a Ru phase with a hexagonal close-packed (hcp) crystal structure. Our observation reveals that the hcp Ru phase forms in two steps: the spinodal decomposition of the alloy produces metastable fcc Ru clusters, and as they grow larger, these clusters transform into hcp Ru domains. Our calculations indicate that the primary reason for the fcc-to-hcp transformation is the size-dependent competition between the interfacial and bulk energies of Ru domains. These insights into elusive, transient steps in the phase separation of alloys can aid in engineering nanomaterials with unconventional phases.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Phase separation plays a crucial role in many natural and industrial processes, such as the formation of clouds and minerals and the distillation of crude oil. In metals and alloys, phase separation is an important approach often utilized to improve their mechanical strength for use in construction, automobile, and aerospace manufacturing. Despite its importance in many processes, the atomic details of phase separation are largely unknown. In particular, it is unclear how a different crystal phase emerges from the parent alloy. Here, using real-time in situ transmission electron microscopy, we describe the stages of the phase separation in face-centered cubic (fcc) AuRu alloy nanoparticles, resulting in a Ru phase with a hexagonal close-packed (hcp) crystal structure. Our observation reveals that the hcp Ru phase forms in two steps: the spinodal decomposition of the alloy produces metastable fcc Ru clusters, and as they grow larger, these clusters transform into hcp Ru domains. Our calculations indicate that the primary reason for the fcc-to-hcp transformation is the size-dependent competition between the interfacial and bulk energies of Ru domains. These insights into elusive, transient steps in the phase separation of alloys can aid in engineering nanomaterials with unconventional phases. |
Carrio, Juan A G; Donato, Ricardo K; Carvalho, Alexandra; Koon, Gavin K W; Donato, Katarzyna Z; Yau, Xin Hui; Kosiachevskyi, Dmytro; Lim, Karen; Ravi, Vedarethinam; Joy, Josny; Goh, Kelda; Emiliano, Jose Vitorio; Lombardi, Jerome E; Neto, Castro A H From 2D kaolinite to 3D amorphous cement Journal Article SCIENTIFIC REPORTS, 15 (1), 2025, ISSN: 2045-2322. Abstract | Links | BibTeX @article{ISI:001396241000050,
title = {From 2D kaolinite to 3D amorphous cement},
author = {Juan A G Carrio and Ricardo K Donato and Alexandra Carvalho and Gavin K W Koon and Katarzyna Z Donato and Xin Hui Yau and Dmytro Kosiachevskyi and Karen Lim and Vedarethinam Ravi and Josny Joy and Kelda Goh and Jose Vitorio Emiliano and Jerome E Lombardi and Castro A H Neto},
doi = {10.1038/s41598-024-81882-1},
times_cited = {0},
issn = {2045-2322},
year = {2025},
date = {2025-01-11},
journal = {SCIENTIFIC REPORTS},
volume = {15},
number = {1},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {Kaolinite is a single 2D layer of kaolin or metakaolin (MK), common clays that can be characterized as layered 3D materials. We show that because of its chemical composition, kaolinite can be converted into an amorphous 3D material by chemical means. This dimensional transformation is possible due to the large surface to volume ratio and chemical reactivity of kaolinite. We investigate the formation and influence of quasi- or nanocrystalline phases in MK-based alkali-activated materials (AAM) that are related to the Si/Al ratio. We analyze the formation of an AAM from a MK precursor, which is a 3D bonded network that preserves the layered structure at the nanometer scale. We also exfoliate the remaining layered phase to examine the effects of the alkali-activation in the final sheet structures embedded within the amorphous network. The final material can be used as a cement with no carbon dioxide produced by the transformation reaction.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Kaolinite is a single 2D layer of kaolin or metakaolin (MK), common clays that can be characterized as layered 3D materials. We show that because of its chemical composition, kaolinite can be converted into an amorphous 3D material by chemical means. This dimensional transformation is possible due to the large surface to volume ratio and chemical reactivity of kaolinite. We investigate the formation and influence of quasi- or nanocrystalline phases in MK-based alkali-activated materials (AAM) that are related to the Si/Al ratio. We analyze the formation of an AAM from a MK precursor, which is a 3D bonded network that preserves the layered structure at the nanometer scale. We also exfoliate the remaining layered phase to examine the effects of the alkali-activation in the final sheet structures embedded within the amorphous network. The final material can be used as a cement with no carbon dioxide produced by the transformation reaction. |
Hao, Qi; Liu, Yijun; Zou, Ren; Shi, Ge; Yang, Shilian; Zhong, Linxin; Yang, Wu; Chi, Xiao; Liu, Yunpeng; Admassie, Shimelis; Peng, Xinwen g-C3N4 nanosheets coupled with CoSe2 as co-catalyst for efficient photooxidation of xylose to xylonic acid Journal Article GREEN ENERGY & ENVIRONMENT, 10 (1), pp. 231-238, 2025, ISSN: 2096-2797. Abstract | Links | BibTeX @article{ISI:001395719700001,
title = {\textit{g}-C_{3}N_{4} nanosheets coupled with CoSe_{2} as co-catalyst for efficient photooxidation of xylose to xylonic acid},
author = {Qi Hao and Yijun Liu and Ren Zou and Ge Shi and Shilian Yang and Linxin Zhong and Wu Yang and Xiao Chi and Yunpeng Liu and Shimelis Admassie and Xinwen Peng},
doi = {10.1016/j.gee.2024.04.004},
times_cited = {0},
issn = {2096-2797},
year = {2025},
date = {2025-01-01},
journal = {GREEN ENERGY & ENVIRONMENT},
volume = {10},
number = {1},
pages = {231-238},
publisher = {KEAI PUBLISHING LTD},
address = {16 DONGHUANGCHENGGEN NORTH ST, Building 5, Room 411, BEIJING, DONGCHENG DISTRICT 100009, PEOPLES R CHINA},
abstract = {Photocatalysis has emerged as an effective approach to sustainably convert biomass into value-added products. CoSe2 is a promising non-precious, efficient cocatalyst for photooxidation, which can facilitate the separation of photogenerated electron-holes, increase the reaction rates, and enhance photocatalytic efficiency. In this work, we synthesized a stable and efficient photocatalysis system of CoSe2/g-C3N4 through attaching CoSe2 on g-C3N4 sheets, with a yield of 50.12% for the selective photooxidation of xylose to xylonic acid. Under light illumination, the photogenerated electrons were prone to migrating from g-C3N4 to CoSe2 due to the higher work function of CoSe2, resulting in the accelerated separation of photogenerated electron-holes and the promoted photooxidation. Herein, this study reveals the unique function of CoSe2, which can significantly promote oxygen adsorption, work as an electron sink and accelerate the generation of center dot O-2, thereby improving the selectivity toward xylonic acid over other by-products. This work provides useful insights into the design of selective photocatalysts by engineering g-C3N4 for biomass high-value utilization. (c) 2025 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co., Ltd.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Photocatalysis has emerged as an effective approach to sustainably convert biomass into value-added products. CoSe2 is a promising non-precious, efficient cocatalyst for photooxidation, which can facilitate the separation of photogenerated electron-holes, increase the reaction rates, and enhance photocatalytic efficiency. In this work, we synthesized a stable and efficient photocatalysis system of CoSe2/g-C3N4 through attaching CoSe2 on g-C3N4 sheets, with a yield of 50.12% for the selective photooxidation of xylose to xylonic acid. Under light illumination, the photogenerated electrons were prone to migrating from g-C3N4 to CoSe2 due to the higher work function of CoSe2, resulting in the accelerated separation of photogenerated electron-holes and the promoted photooxidation. Herein, this study reveals the unique function of CoSe2, which can significantly promote oxygen adsorption, work as an electron sink and accelerate the generation of center dot O-2, thereby improving the selectivity toward xylonic acid over other by-products. This work provides useful insights into the design of selective photocatalysts by engineering g-C3N4 for biomass high-value utilization. (c) 2025 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co., Ltd. |
Carrio, Juan A G; Talluri, Vssl Prasad; Toolahalli, Swamy T; Echeverrigaray, Sergio G; Neto, Antonio Castro H Cross-Linked Self-Standing Graphene Oxide Membranes: A Pathway to Scalable Applications in Separation Technologies Journal Article MEMBRANES, 15 (1), 2025. Abstract | Links | BibTeX @article{ISI:001404434600001,
title = {Cross-Linked Self-Standing Graphene Oxide Membranes: A Pathway to Scalable Applications in Separation Technologies},
author = {Juan A G Carrio and Vssl Prasad Talluri and Swamy T Toolahalli and Sergio G Echeverrigaray and Antonio Castro H Neto},
doi = {10.3390/membranes15010031},
times_cited = {0},
year = {2025},
date = {2025-01-01},
journal = {MEMBRANES},
volume = {15},
number = {1},
publisher = {MDPI},
address = {ST ALBAN-ANLAGE 66, CH-4052 BASEL, SWITZERLAND},
abstract = {The large-scale implementation of 2D material-based membranes is hindered by mechanical stability and mass transport control challenges. This work describes the fabrication, characterisation, and testing of self-standing graphene oxide (GO) membranes cross-linked with oxides such as Fe2O3, Al2O3, CaSO4, Nb2O5, and a carbide, SiC. These cross-linking agents enhance the mechanical stability of the membranes and modulate their mass transport properties. The membranes were prepared by casting aqueous suspensions of GO and SiC or oxide powders onto substrates, followed by drying and detachment to yield self-standing films. This method enabled precise control over membrane thickness and the formation of laminated microstructures with interlayer spacings ranging from 0.8 to 1.2 nm. The resulting self-standing membranes, with areas between 0.002 m2 and 0.090 m2 and thicknesses from 0.6 mu m to 20 mu m, exhibit excellent flexibility and retain their chemical and physical integrity during prolonged testing in direct contact with ethanol/water and methanol/water mixtures in both liquid and vapour phases, with stability demonstrated over 24 h and up to three months. Gas permeation and chemical characterisation tests evidence their suitability for gas separation applications. The interactions promoted by the oxides and carbide with the functional groups of GO confer great stability and unique mass transport properties-the Nb2O5 cross-linked membranes present distinct performance characteristics-creating the potential for scalable advancements in cross-linked 2D material membranes for separation technologies.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The large-scale implementation of 2D material-based membranes is hindered by mechanical stability and mass transport control challenges. This work describes the fabrication, characterisation, and testing of self-standing graphene oxide (GO) membranes cross-linked with oxides such as Fe2O3, Al2O3, CaSO4, Nb2O5, and a carbide, SiC. These cross-linking agents enhance the mechanical stability of the membranes and modulate their mass transport properties. The membranes were prepared by casting aqueous suspensions of GO and SiC or oxide powders onto substrates, followed by drying and detachment to yield self-standing films. This method enabled precise control over membrane thickness and the formation of laminated microstructures with interlayer spacings ranging from 0.8 to 1.2 nm. The resulting self-standing membranes, with areas between 0.002 m2 and 0.090 m2 and thicknesses from 0.6 mu m to 20 mu m, exhibit excellent flexibility and retain their chemical and physical integrity during prolonged testing in direct contact with ethanol/water and methanol/water mixtures in both liquid and vapour phases, with stability demonstrated over 24 h and up to three months. Gas permeation and chemical characterisation tests evidence their suitability for gas separation applications. The interactions promoted by the oxides and carbide with the functional groups of GO confer great stability and unique mass transport properties-the Nb2O5 cross-linked membranes present distinct performance characteristics-creating the potential for scalable advancements in cross-linked 2D material membranes for separation technologies. |