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Balance between FeIV-NiIV synergy and Lattice Oxygen Contribution for Accelerating Water Oxidation

ACS Nano 2024年第22期18卷 14496-14506页

作者： Jing, Chao Li, Lili Chin, Yi-Ying Pao, Chih-Wen Huang, Wei-Hsiang Liu, Miaomiao Zhou, Jing Yuan, Taotao Zhou, Xiangqi Wang, Yifeng Chen, Chien-Te Li, Da-Wei Wang, Jian-Qiang Hu, Zhiwei Zhang, Linjuan Key Laboratory of Interfacial Physics and Technology Shanghai Institute of Applied Physics Chinese Academy of Sciences Jialuo Road 2019 Shanghai201800 China School of Chemistry & Molecular Engineering East China University of Science and Technology 130 Meilong Road Shanghai200237 China Max Planck Institute for Chemical Physics of Solids Nöthnitzer Strasse 40 Dresden01187 Germany State Key Laboratory of Crystal Materials and Institute of Crystal Materials Shandong University Jinan250100 China Department of Physics National Chung Cheng University Chiayi621301 Taiwan National Synchrotron Radiation Research Center 101 Hsin-Ann Road Hsinchu300092 Taiwan Zhejiang Institute of Photoelectronics & Zhejiang Institute for Advanced Light Source Zhejiang Normal University Zhejiang Jinhua321004 China University of Chinese Academy of Sciences Beijing100049 China

Hydrogen obtained from electrochemical water splitting is the most promising clean energy carrier, which is hindered by the sluggish kinetics of the oxygen evolution reaction (OER). Thus, the development of an efficient OER electrocatalyst using nonprecious 3d transition elements is desirable. Multielement synergistic effect and lattice oxygen oxidation are two well-known mechanisms to enhance the OER activity of catalysts. The latter is generally related to the high valence state of 3d transition elements leading to structural destabilization under the OER condition. We have found that Al doping in nanosheet Ni-Fe hydroxide exhibits 2-fold advantage: (1) a strong enhanced OER activity from 277 mV to 238 mV at 10 mA cm-2 as the Ni valence state increases from Ni3.58+ to Ni3.79+ observed from in situ X-ray absorption spectra. (2) Operational stability is strengthened, while weakness is expected since the increased NiIV content with 3d8L2 (L denotes O 2p hole) would lead to structural instability. This contradiction is attributed to a reduced lattice oxygen contribution to the OER upon Al doping, as verified through in situ Raman spectroscopy, while the enhanced OER activity is interpreted as an enormous gain in exchange energy of FeIV-NiIV, facilitated by their intersite hopping. This study reveals a mechanism of Fe-Ni synergy effect to enhance OER activity and simultaneously to strengthen operational stability by suppressing the contribution of lattice oxygen. © 2024 The Authors. Published by American chemical Society.

关键词： Oxygen

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Subaqueous Acoustic Pressure System Based One Day Heterotypic Pseudo-Islet Spheroid Formation with Adipose Derived Stem Cells for Graft Survival-Related Function Enhancement

SSRN

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SSRN 2025年

作者： Hyun, Jiyu Park, Junhyeung Song, Jihun Yoo, Chae Rim Jang, Seon Mi Lee, Sang Yoon Jung, Seunghyuk Lee, Tae Il Park, Ki Dong Jeong, Jee-Heon Park, Hyun-Ji Lee, Dong Yun Bhang, Suk Ho School of Chemical Engineering Sungkyunkwan University Suwon16419 Korea Republic of Department of Precision Medicine School of Medicine Sungkyunkwan University Suwon16419 Korea Republic of Department of Biomedical Sciences Seoul National University Hospital Seoul National University College of Medicine Seoul03080 Korea Republic of Department of Bioengineering College of Engineering BK FOUR Biopharmaceutical Innovation Leader for Education and Research Group Hanyang University Seoul04763 Korea Republic of Department of Molecular Science and Technology Ajou University Suwon16499 Korea Republic of Department of Materials Science and Engineering Gachon University Seong-nam 13120 Korea Republic of Advanced College of Bio-Convergence Engineering Ajou University Suwon16499 Korea Republic of

To overcome Type 1 diabetes mellitus (T1DM), which can cause hyperglycemia due to diminished insulin secretion of β-cell function, islet transplantation has been developed with various strategies including pseudo-islet. However, conventional pseudo-islet formation techniques combining with other cells depend on natural cellular aggregation, which requires at least 5 days to form and even show segregation of distinct cell types, leading to diminished cell viability and function. Herein, we applied a subaqueous free-standing 3D cell culture (FS) device, which can reduce the spheroid formation by trapped cell in nodes of acoustic standing wave. Briefly, Culturing with adipose-derived stem cells (ADSCs) to form heterotypic pseudo-islet (Hislet) in FS device dramatically reduced formation time less than one day. Hislet demonstrated enhancement of cell viability than conventional pseudo-islet formation method. Additionally, ADSCs combined Hislet proved strong secretion of various paracrine factors. Also results showed significantly increased angiogenesis effect and M1-to-M2 transition of macrophages in Hislet compared to islet, which can enhance transplantation survival. Furthermore, Hislet maintain glucose-responsive insulin secretion and exhibit high durability without any segregation in harsh condition that mimic transplantation environment. Throughout this study, we propose a novel strategy for forming Hislet that can overcome the limitations of conventional islets and pseudo-islets. © 2025, The Authors. All rights reserved.

关键词： Stem cells

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Boron nitride for enhanced oxidative dehydrogenation of ethylbenzene

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Journal of Energy Chemistry 2021年第6期30卷 477-484,I0012页

作者： Rui Han Jiangyong Diao Sonu Kumar Andrey Lyalin Tetsuya Taketsugu Gilberto Casillas Christopher Richardson Feng Liu Chang Won Yoon Hongyang Liu Xudong Sun Zhenguo Huang Key Laboratory for Anisotropy and Texture of Materials(Ministry of Education) Northeastern UniversityShenyang 110819LiaoningChina School of Civil and Environmental Engineering University of Technology SydneyUltimoNew South Wales 2007Australia Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina Institute for Chemical Reaction Design and Discovery(WPI-ICReDD) Hokkaido UniversitySapporo 001-0021Japan Center for Green Research on Energy and Environmental Materials National Institute for Materials Science(NIMS)Tsukuba 305-0044Japan Department of Chemistry Faculty of ScienceHokkaido UniversitySapporo 060-0810Japan Electron Microscopy Centre University of WollongongNew South Wales 2500Australia Molecular Horizons and School of Chemistry and Molecular Bioscience Faculty of ScienceMedicine and HealthUniversity of WollongongNew South Wales 2522Australia Center for Hydrogen and Fuel Cell Research Korea Institute of Science and TechnologySeoul 02792Republic of Korea

It is demonstrated experimentally and confirmed theoretically that highly defective boron nitride showed outstanding performance for oxidative dehydrogenation of *** catalyst is derived from carbon-doped hexagonal boron nitride nanosheets synthesized via a two-step reaction when participating the oxidative dehydrogenation *** first step yields a polymeric precursor with the atomic positions of B,C,N relatively constrained,which is conducive for the formation of carbon atomic clusters uniformly dispersed throughout the BN *** the oxidative dehydrogenation of ethylbenzene to styrene,the nanoscale carbon clusters are removed and highly defective boron nitride(D-BN)is obtained,exposing boron-rich zigzag edges of BN that act as the catalytic *** catalytic performance of D-BN is therefore remarkably better than un-doped *** results indicate that dispersed C-doping in h-BN is highly effective in terms of defect formation and resultant enhanced activity in oxidative dehydrogenation reactions.

关键词： Boron nitride Dehydrogenation Ethylbenzene Carbon-doping Heterogeneous catalysis

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Sub-femtonewton force sensing in solution by super-resolved photonic force microscopy (Jun, 10.1038/s41566-024-01462-7, 2024)

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NATURE PHOTONICS 2024年第9期18卷 998-998页

作者： Shan, Xuchen Ding, Lei Wang, Dajing Wen, Shihui Shi, Jinlong Chen, Chaohao Wang, Yang Zhu, Hongyan Huang, Zhaocun Wang, Shen S. J. Zhong, Xiaolan Liu, Baolei Reece, Peter John Ren, Wei Hao, Weichang Lu, Xunyu Lu, Jie Su, Qian Peter Chang, Lingqian Sun, Lingdong Jin, Dayong Jiang, Lei Wang, Fan School of Physics Beihang University Beijing People’s Republic of China Science and Technology Center for Quantum Biology National Institute of Extremely-Weak Magnetic Field Infrastructure Hangzhou People’s Republic of China School of Biomedical Engineering Faculty of Engineering and Information Technology University of Technology Sydney Sydney New South Wales Australia Centre for Atomaterials and Nanomanufacturing School of Science RMIT University Melbourne Victoria Australia Institute for Biomedical Materials and Devices (IBMD) School of Mathematical and Physical Sciences Faculty of Science University of Technology Sydney Sydney New South Wales Australia Eastern Institute for Advanced Study Eastern Institute of Technology Ningbo People’s Republic of China Key Laboratory of Bio-Inspired Materials and Interfaces Sciences Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing People’s Republic of China Australian Research Council Centre of Excellence for Transformative Meta-Optical Systems Department of Electronic Materials Engineering Research School of Physics The Australian National University Canberra Australian Capital Territory Australia Key Laboratory of Biomechanics and Mechanobiology (Ministry of Education) Beijing Advanced Innovation Center for Biomedical Engineering School of Biological Science and Medical Engineering Beihang University Beijing People’s Republic of China Computing and Information Systems Department Melbourne School of Engineering University of Melbourne Melbourne Victoria Australia School of Physics The University of New South Wales Sydney New South Wales Australia School of Chemistry & Chemical Engineering Shaanxi Normal University Xi’an People’s Republic of China Particles and Catalysis Research Laboratory School of Chemical Engineering The University of New South Wales Sydney New South Wales Australia Australian Artificial Intelligence Institute Faculty of Engineering and IT University of Technology

Precise force measurement is critical to probe biological events and physics processes, spanning from molecular motor’s motion to the Casimir effect, as well as the detection of gravitational waves. Yet, despite extensive technological developments, the three-dimensional nanoscale measurement of weak forces in aqueous solutions still faces major challenges. Techniques that rely on optically trapped nanoprobes are of significant potential but are beset with limitations, including probe heating induced by high trapping power, undetectable scattering signals and localization errors. Here we report the measurement of the long-distance interaction force in aqueous solutions with a minimum detected force value of 108.2 ± 510.0 attonewton. To achieve this, we develop a super-resolved photonic force microscope based on optically trapped lanthanide-doped nanoparticles coupled with nanoscale three-dimensional tracking-based force sensing. The tracking method leverages neural-network-empowered super-resolution localization, where the position of the force probe is extracted from the optical-astigmatism-modified point spread function. We achieve a force sensitivity down to 1.8 fN Hz–1/2, which approaches the nanoscale thermal limit. We experimentally measure electrophoresis forces acting on single nanoparticles as well as the surface-induced interaction force on a single nanoparticle. This work opens the avenue of nanoscale thermally limited force sensing and offers new opportunities for detecting sub-femtonewton forces over long distances and biomechanical forces at the single-molecule level.

关键词： Electrophoresis

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Accelerated Discovery of Solvation Structure engineering for Stable Aqueous Rechargeable Zinc Batteries via Physics-Guided Bayesian Active Learning (Small 23/2025)

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Small 2025年第23期21卷

作者： Minsu Kim Minji Lee Inyoung Choi Jihye Oh Sanga Paik Areum Han Sinae Lee Hyerim Hwang Jonggeol Na Kwan Woo Nam Department of Chemical Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA Department of Chemical Engineering and Materials Science Graduate Program in System Health Science and Engineering Ewha Womans University Seoul 03760 Republic of Korea

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Coherent Acoustic Phonons in Bi2Se3 Ultrathin Films Probed by Femtosecond, Optical Pump-Probe Spectroscopy

Coherent Acoustic Phonons in Bi2Se3 Ultrathin Films Probed b...

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CLEO: Fundamental science, CLEO:FS 2024 - Part of Conference on Lasers and Electro-Optics, CLEO 2024

作者： Cheng, Jing Niherysh, Kiryl A. Francis, Peter Chakraborty, Debamitra Lombardi, Floriana Erts, Donats Prischepa, Serghej L. Laszcz, Adam Komissarov, Ivan V. Sobolewski, Roman Materials Science Graduate Program University of Rochester RochesterNY14627 United States Laboratory for Laser Energetics University of Rochester RochesterNY14623-1299 United States Department of Microtechnology and Nanoscience Chalmers University of Technology Gothenburg Sweden Institute of Chemical Physics University of Latvia Riga Latvia Department of Electrical and Computer Engineering University of Rochester RochesterNY14627 United States Dipartimento di Fisica "E.R. Caianiello" Università degli Studi di Salerno Sa FiscianoI-84084 Italy Lukasiewicz Research Network Institute of Microelectronics and Photonics WarszawaPL-02668 Poland

ISBN: (纸本)9781957171395

The dynamics of coherent acoustic phonons in the Bi2Se3 layered crystal system are investigated. The findings reveal that the frequency evolution of breathing modes with the number of the material quintuple layers and the dispersion relation both can be explained by a modified chain model with a nonuniform coupling force. © Optica Publishing Group 2024, © 2024 The Author(s)

关键词： Ultrathin films

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One Set to Rule Them All: How to Obtain General chemical Conditions via Bayesian Optimization over Curried Functions

arXiv

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arXiv 2025年

作者： Schmid, Stefan P. Rajaonson, Ella Miray Ser, Cher Tian Haddadnia, Mohammad Leong, Shi Xuan Aspuru-Guzik, Alán Kristiadi, Agustinus Jorner, Kjell Strieth-Kalthoff, Felix Institute of Chemical and Bioengineering Department of Chemistry and Applied Biosciences ETH Zurich ZurichCH-8093 Switzerland Catalysis ETH Zurich ZurichCH-8093 Switzerland Department of Chemistry University of Toronto Toronto Canada Vector Institute Toronto Canada Department of Biological Chemistry & Molecular Pharmacology Harvard University CambridgeMA United States Dana-Farber Cancer Institute BostonMA United States School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University Singarpore Singapore Department of Computer Science University of Toronto Toronto Canada Department of Chemical Engineering and Applied Chemistry University of Toronto Toronto Canada Department of Materials Science and Engineering University of Toronto Toronto Canada Acceleration Consortium University of Toronto Toronto Canada Canada School of Mathematics and Natural Sciences University of Wuppertal Wuppertal Germany

General parameters are highly desirable in the natural sciences — e.g., chemical reaction conditions that enable high yields across a range of related transformations. This has a significant practical impact since those general parameters can be transferred to related tasks without the need for laborious and time-intensive re-optimization. While Bayesian optimization (BO) is widely applied to find optimal parameter sets for specific tasks, it has remained underused in experiment planning towards such general optima. In this work, we consider the real-world problem of condition optimization for chemical reactions to study how performing generality-oriented BO can accelerate the identification of general optima, and whether these optima also translate to unseen examples. This is achieved through a careful formulation of the problem as an optimization over curried functions, as well as systematic evaluations of generality-oriented strategies for optimization Copyright © 2025, The Authors. All rights reserved.

关键词：

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Directly freeze-drying porous graphene aerogel as acoustic-absorbing material 3

Directly freeze-drying porous graphene aerogel as acoustic-a...

引用

2021 3rd International Conference on Polymer Synthesis and Application, ICPSA 2021

作者： Li, Zengling Chen, Nan Qu, Liangti Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials Key Laboratory of Cluster Science Ministry of Education of China School of Chemistry and Chemical Engineering Beijing Institute of Technology Beijing100081 China Key Laboratory of Organic Optoelectronics and Molecular Engineering Ministry of Education Department of Chemistry Tsinghua University Beijing100084 China

Noise pollution, which is no less harmful than air, water and soil pollution, is becoming an environmental shortcoming that cannot be ignored. Scientists are also seeking various solutions to work on reducing noise pollution. In this work, porous graphene aerogel (FD-GA) and porous graphene oxide aerogel (FD-GOA) prepared by foaming combined with freeze-drying are reported as acoustic-absorbing materials. The effects of thickness and degree of compression on the acoustic-absorbing performance of FD-GA and FD-GOA in the 1000- 6000 Hz range, where human ear hearing is sensitive, were investigated, respectively. FD-GA was found to have significantly higher acoustic absorption performance with a peak absorption of 96.7%. The present work provides a simple and straightforward strategy for the synthesis of the acoustic-absorbing material. Key words: freeze-drying, graphene aerogel, acousticabsorbing. © 2021 Institute of Physics Publishing. All rights reserved.

关键词： Noise pollution

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Room-temperature multiple ligands-tailored SnO_(2) quantum dots endow in situ dual-interface binding for upscaling efficient perovskite photovoltaics with high V_(OC)

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Light(science & Applications) 2021年第12期10卷 2467-2481页

作者： Zhiwei Ren Kuan Liu Hanlin Hu Xuyun Guo Yajun Gao Patrick W.K.Fong Qiong Liang Hua Tang Jiaming Huang Hengkai Zhang Minchao Qin Li Cui Hrisheekesh Thachoth Chandran Dong Shen Ming-Fai Lo Annie Ng Charles Surya Minhua Shao Chun-Sing Lee Xinhui Lu Frédéric Laquai Ye Zhu Gang Li Department of Electronic and Information Engineering Research Institute for Smart Energy(RISE)Guangdong-Hong Kong-Macao(GHM)Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and DevicesThe Hong Kong Polytechnic UniversityHung HomKowloonHong KongChina Department of Electrical and Computer Engineering Nazarbayev UniversityNur-SultanKazakhstan The Hong Kong Polytechnic University Shenzhen Research Institute Shenzhen 518057China Hoffmann Institute of Advanced Materials Shenzhen Polytechnic7098 Liuxian BoulevardShenzhen 518055China Department of Applied Physics The Hong Kong Polytechnic UniversityHung HomKowloonHong KongChina Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina King Abdullah University of Science and Technology(KAUST) KAUST Solar Center(KSC)Physical Sciences and Engineering Division(PSE)Material Science and Engineering Program(MSE)Thuwal 23955-6900Kingdom of Saudi Arabia Department of Physics The Chinese University of Hong KongShatin 999077 Hong KongChina Center of Super-Diamond and Advanced Films(COSDAF) Department of ChemistryCity University of Hong KongHong KongChina

The benchmark tin oxide(SnO_(2))electron transporting layers(ETLs)have enabled remarkable progress in planar perovskite solar cell(PSCs).However,the energy loss is still a challenge due to the lack of“hidden interface”*** report a novel ligand-tailored ultrafine SnO_(2) quantum dots(QDs)via a facile rapid room temperature ***,the ligand-tailored SnO_(2) QDs ETL with multi-functional terminal groups in situ refines the buried interfaces with both the perovskite and transparent electrode via enhanced interface binding and perovskite *** novel ETLs induce synergistic effects of physical and chemical interfacial modulation and preferred perovskite crystallization-directing,delivering reduced interface defects,suppressed non-radiative recombination and elongated charge carrier *** conversion efficiency(PCE)of 23.02%(0.04 cm^(2))and 21.6%(0.98 cm^(2),V_(OC) loss:0.336 V)have been achieved for the blade-coated PSCs(1.54 eV E_(g))with our new ETLs,representing a record for SnO_(2) based blade-coated ***,a substantially enhanced PCE(V_(OC))from 20.4%(1.15 V)to 22.8%(1.24 V,90 mV higher V_(OC),0.04 cm^(2) device)in the blade-coated 1.61 eV PSCs system,via replacing the benchmark commercial colloidal SnO_(2) with our new ETLs.

关键词： perovskite interface quantum

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Recent advances in self-immobilizing fluorescent probes for in vivo imaging

Smart Molecules

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Smart Molecules 2024年第3期2卷 39-52页

作者： Yong Zhang Xuemei Lv Yafu Wang Xueqian Chen Jinchao Zhang Dongdong Su State Key Laboratory of New Pharmaceutical Preparations and Excipients Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of Ministry of EducationCollege of Chemistry&Materials ScienceChemical Biology Key Laboratory of Hebei ProvinceHebei UniversityBaodingChina School of Chemistry and Chemical Engineering Henan Normal UniversityXinxiangHenanChina Department of Chemistry Center of Excellence for Environmental Safety and Biological EffectsBeijing Key Laboratory for Green Catalysis and SeparationBeijing University of TechnologyBeijingChina

In situ precise detection of bioactive molecules with high sensitivity and spatiotemporal resolution is essential for studying physiological events and disease *** utilization of versatile fluorescent probes in fluorescence imaging offers a powerful tool for in vivo imaging of biomarkers closely associated with pathological ***,the dynamic behavior leading to rapid clearance of small molecule probes from regions of interest severely compromises their potential for precise ***,self-immobilizing fluorescent probes that selectively recognize diseased tissues while improving in situ retention and enrichment enable accurate high-fidelity fluorescence *** this review,we aim to summarize the strategies employed for recent advances in the performance and precision of in vivo fluorescence imaging using self-immobilizing ***,we discuss the prospects and potential challenges associated with selfimmobilizing fluorescent probes to promote further development and application of more delicate fluorescent probes.

关键词： biomarkers fluorescent probes in situ precise imaging self-immobilizing

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