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Synthesis of Iron-Carbide Nanoparticles:Identification of the Active Phase and Mechanism of Fe-Based Fischer-Tropsch Synthesis

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CCS Chemistry 2021年第11期3卷 2712-2724页

作者： Huabo Zhao Jin-Xun Liu Ce Yang Siyu Yao Hai-Yan Su Zirui Gao Mei Dong Junhu Wang Alexandre I.Rykov Jianguo Wang Yanglong Hou Wei-Xue Li Ding Ma College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871 Department of Chemical Physics School of Chemistry and Materials ScienceHefei National Laboratory for Physical Sciences at the MicroscaleiCHEMUniversity of Science and Technology of ChinaHefei 230026 Department of Materials Science and Engineering College of EngineeringPeking UniversityBeijing 100871 School of Chemical Engineering and Energy Technology Dongguan University of TechnologyDongguan 523808 State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001 Center for Advanced Mössbauer Spectroscopy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023

Despite the extensive study of the Fe-based Fischer-Tropsch synthesis(FTS)over the past 90 years,its active phases and reaction mechanisms are still unclear due to the coexistence of metals,oxides,and carbide phases presented under realistic FTS reaction conditions and the complex reaction network involving CO activation,C-C coupling,and methane *** address these issues,we successfully synthesized a range of pure-phase iron and iron-carbide nanoparticles(Fe,Fe_(5)C_(2),Fe_(3)C,and Fe_(7)C_(3))for the first *** using them as the ideal model catalysts on high-pressure transient experiments,we identified unambiguously that all the iron carbides are catalytically active in the FTS reaction while Fe_(5)C_(2) is the most active yet stable carbide phase,consistent with density functional theory(DFT)calculation *** reaction mechanism and kinetics of Fe-based FTS were further explored on the basis of those model catalysts by means of transient high-pressure stepwise temperature-programmed surface reaction(STPSR)experiments and DFT *** work provides new insights into the active phase of iron carbides and corresponding FTS reaction mechanism,which is essential for better iron-based catalyst design for FTS reactions.

关键词： Fischer-Tropsch synthesis iron carbides active phase reaction mechanism

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Uncovering interfacial electron transfer kinetics of WO₃ biophotoelectrodes for food waste treatment

RSC Applied Interfaces

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RSC Applied Interfaces 2024年第2期2卷 397-409页

作者： Mak, Chun Hong Peng, Yong Chong, Man Hin Mou, Jinhua Jia, Guohua Santoso, Shella Permatasari Niu, Wenxin Lee, Duu-Jong Yu, Chang-Ping Lin, Carol Sze Ki Hsu, Hsien-Yi School of Energy and Environment City University of Hong Kong Kowloon Tong Hong Kong Department of Materials Science and Engineering City University of Hong Kong Kowloon Tong Hong Kong Department of Mechanical Engineering City University of Hong Kong Kowloon Tong Hong Kong Centre for Functional Photonics (CFP) City University of Hong Kong Kowloon Tong Hong Kong Shenzhen Research Institute City University of Hong Kong Shenzhen 518057 China Curtin Institute of Functional Molecules and Interfaces School of Molecular and Life Sciences Curtin University GPO Box U1987 Perth 6845 WA Australia Department of Chemical Engineering Faculty of Engineering Widya Mandala Surabaya Catholic University Kalijudan No. 37 East Java Surabaya 60114 Indonesia State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences 5625 Renmin Street Jilin 130022 Changchun China Graduate Institute of Environmental Engineering National Taiwan University Taipei 10617 Taiwan

An effective approach to enhance bioelectrochemical systems' performance involves leveraging semiconductors' light-harvesting capabilities alongside the catalytic properties of bacteria. Here, we demonstrate a food waste removal method using the integration of Shewanella oneidensis MR-1 with a tungsten(vi) oxide (WO₃) nanoplate photoanode in a solar-assisted microbial photoelectrochemical cell (S-MPEC) combined with silicon-based photovoltaics (SiPV). The S-MPEC integrates the technologies of bioelectrochemical cells with photoelectrochemical cells (PEC) to enhance the degradation of food waste. The bare WO₃ photoelectrode exhibits a photocurrent of 0.749 A m⁻² at 0.8 V under visible light, whereas the WO₃-MR-1 biophotoelectrode reveals a significantly higher photocurrent of 2.94 A m⁻². Under visible light exposure at an intensity of less than 100 mW cm⁻², the power densities of the WO₃ photoelectrode with and without MR-1 bacterial coating are 2.36 W m⁻² and 0.599 W m⁻², respectively. To further improve performance, the S-MPEC was connected with a SiPV. This combined system, PV-S-MPEC, achieved a power density of 21.99 W m⁻² and a chemical oxygen demand (COD) removal rate of 8167 mg L⁻¹ per day, demonstrating its effectiveness in degrading food waste hydrolysate. Additionally, the study of heterogeneous electron transfer kinetics indicated that the WO₃-MR-1 system exhibits more efficient diffusion coefficients and enhanced rate constants for reduction and oxidation reactions. These findings highlight the significant impact of photoexcited charge carriers on degradation performance in this complex hybrid electricigen system, underscoring its potential for developing S-MPECs for waste degradation. This study also demonstrates significant potential for reducing environmental impact through enhanced COD removal rates and energy-efficient w

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Optimizing cyanobacterial hydrogen production: metabolic and genetic strategies with glycerol supplementation

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Frontiers in Energy Research 2025年 13卷

作者： Bozieva, Ayshat M. Khasimov, Makhmadyusuf K. Rao, Mahipal S. Sinetova, Maria A. Voloshin, Roman A. Dunikov, Dmitry O. Tsygankov, Anatoly A. Leong, Yoong Kit Chang, Jo-Shu Allakhverdiev, Suleyman I. Bruce, Barry D. K.A. Timiryazev Institute of Plant Physiology Russian Academy of Sciences Moscow Russia Institute of Basic Biological Problems Russian Academy of Sciences Pushchino Moscow Russia Department of Biochemistry and Cellular and Molecular Biology University of Tennessee KnoxvilleTN United States Laboratory for Hydrogen Energy Technologies Joint Institute for High Temperatures of the Russian Academy of Sciences Moscow Russia Moscow Power Engineering Institute National Research University Moscow Russia Department of Chemical and Materials Engineering Tunghai University Taichung Taiwan Research Center for Smart Sustainable Circular Economy Tunghai University Taichung Taiwan Department of Chemical Engineering National Cheng Kung University Tainan Taiwan Department of Chemical Engineering and Materials Science Yuan Ze University Chung-Li Taiwan Faculty of Engineering and Natural Sciences Bahçeşehir University Istanbul Turkey Department of Chemical and Biomolecular Engineering University of Tennessee KnoxvilleTN United States Department of Microbiology University of Tennessee KnoxvilleTN United States

Introduction: Developing sustainable hydrogen production is critical for advancing renewable energy and reducing reliance on fossil fuels. Cyanobacteria, which harness solar energy through photosynthesis, provide a promising biological platform for hydrogen generation. However, improving hydrogen yields requires strategic metabolic and genetic modifications to optimize energy flow and overcome photosynthetic limitations. Methods: Four cyanobacterial species were evaluated for their hydrogen production capacities under varying experimental conditions. Photosynthesis was partially inhibited using distinct chemical inhibitors, including 3-(3,4-dichlorophenyl)-1,1-dimethylurea (DCMU). Exogenous glycerol was introduced as a supplementary carbon source. Hydrogen production was monitored over time, and rates were normalized to chlorophyll a content. Genomic analysis of transporter proteins was conducted to identify potential genetic loci for further enhancement of hydrogen output. Results: Nitrogen-fixing Dolichospermum sp. exhibited significantly higher hydrogen production compared to the other tested species. Supplementation with glycerol notably increased both the rate and duration of hydrogen evolution, far exceeding previously established benchmarks. The maximum hydrogen production rate for Dolichospermum sp. reached 132.3 μmol H₂/mg Chl a/h—representing a 30-fold enhancement over the rates observed with DCMU. Genomic screening revealed key transporter proteins with putative roles in carbon uptake and hydrogen metabolism. Discussion: These findings underscore the potential of cyanobacteria, particularly Dolichospermum sp., as robust platforms for sustainable hydrogen production. The substantial improvements in hydrogen yield highlight the importance of targeted metabolic engineering and carbon supplementation strategies. Future work focused on optimizing identified transporter proteins and refining genetic interventions could further enhance biohydrogen efficiency. By

关键词： Nitrogen fixation

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Novel polypeptide composite fibrous scaffold with internal chemical boundary

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Journal of Polymer Research 2023年第8期30卷 312-312页

作者： Yang, Shao-Jiun Yu, Tzu-Yi Yu, Jia-Shing Huang, Yu-Ching Lin, Meng-Fang Su, Wei-Fang Department of Materials Science and Engineering National Taiwan University Taipei10617 Taiwan Department of Chemical Engineering National Taiwan University Taipei10617 Taiwan Molecular Image Center National Taiwan University Taipei10617 Taiwan Department of Materials Engineering Ming-Chi University of Technology New Taipei City243303 Taiwan Biochemical Technology R&D Center Ming-Chi University of Technology New Taipei City243303 Taiwan

Cell migration determines the complete development of mammalian tissue and other pathological phenomena. To investigate the effect of chemical stimuli on such behavior, cells are triggered to translate by the concentration gradient of different molecules on 2D substrates in vitro. But to date unfortunately the polymeric scaffolds for cell migration in 3D environment with chemical stimuli have not been proposed and developed yet. Herein, a novel 3D composite scaffold with an internal chemical boundary is fabricated by electrospinning and mask-assisted electrospray so that the deposition of PBG-N3 particles is confined at specific area initially. The chemical boundary is subsequently formed after selective surface modification of the particles via click reaction. Using a fluorescent alkyne, the boundary of modified regions is clearly observed by fluorescence microscope. This innovative bio-material has the potential to serve as a promising scaffold for investigating the effect of chemical stimuli on cell migration and growth in 3D environment and further on to the application in tissue engineering. © 2023, The Polymer Society, Taipei.

关键词： Fluorescence

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Single-Layer Hexagonal Boron Nitride Nanopores as High-Performance Ionic Gradient Power Generators

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Small 2024年第16期20卷 2306018-2306018页

作者： Liu, Ting-Ran Fung, Man Yui Thomas Yeh, Li-Hsien Chiang, Chun-Hao Yang, Jhih-Sian Kuo, Pai-Chia Shiue, Jessie Chen, Chia-Chun Chen, Chun-Wei Department of Materials Science and Engineering National Taiwan University Taipei10617 Taiwan Department of Chemical Engineering National Taiwan University of Science and Technology Taipei10607 Taiwan Advanced Manufacturing Research Center National Taiwan University of Science and Technology Taipei10607 Taiwan Department of Chemistry National Taiwan Normal University Taipei11677 Taiwan Institute of Atomic and Molecular Science Academia Sinica Taipei10617 Taiwan Center of Condensed Matter Science National Taiwan University Taipei10617 Taiwan National Taiwan University Taipei10617 Taiwan

Atomically thin two-dimensional (2D) materials have emerged as promising candidates for efficient energy harvesting from ionic gradients. However, the exploration of robust 2D atomically thin nanopore membranes, which hold sufficient ionic selectivity and high ion permeability, remains challenging. Here, the single-layer hexagonal boron nitride (hBN) nanopores are demonstrated as various high-performance ion-gradient nanopower harvesters. Benefiting from the ultrathin atomic thickness and large surface charge (also a large Dukhin number), the hBN nanopore can realize fast proton transport while maintaining excellent cation selectivity even in highly acidic environments. Therefore, a single hBN nanopore achieves the pure osmosis-driven proton-gradient power up to ≈3 nW under 1000-fold ionic gradient. In addition, the robustness of hBN membranes in extreme pH conditions allows the ionic gradient power generation from acid-base neutralization. Utilizing 1 m HCl/KOH, the generated power can be promoted to an extraordinarily high level of ≈4.5 nW, over one magnitude higher than all existing ionic gradient power generators. The synergistic effects of ultrathin thickness, large surface charge, and excellent chemical inertness of 2D single-layer hBN render it a promising membrane candidate for harvesting ionic gradient powers, even under extreme pH conditions. © 2023 Wiley-VCH GmbH.

关键词： III-V semiconductors

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Fast water transport and ionic sieving in ultrathin stacked nanoporous 2D membranes

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National science Review 2025年第3期 316-324页

作者： Jingfeng Wang Xiaoming Zhang Zehua Yu Yuyan Gao Qingqing Lu Chao Ma Kang Liu Quan Yuan Yanbing Yang College of Chemistry and Molecular Sciences Key Laboratory of Biomedical Polymers of Ministry of Education School of Power and Mechanical Engineering Institute of Molecular Medicine Renmin Hospital of Wuhan University School of Microelectronics Wuhan University Department of Engineering Science and Mechanics The Pennsylvania State University Molecular Science and Biomedicine Laboratory (MBL) State Key Laboratory of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical Engineering College of Materials Science and Engineering Hunan University

Atomically thin nanoporous 2D membranes, featuring unique sieving characteristics for molecules and ions,have significant potential for seawater desalination. However, they face a common trade-off between permeability and selectivity. Here, we report an ultrathin stacked nanoporous graphene membrane(SNGM) created by layering atomically thin graphene nanomesh. This design achieves highly efficient and selective sieving of water molecules and ions. The SNGMs showcase in-plane nanopores for optimal size-exclusive water input and output, and interlayer 2D nanochannels between adjacent graphene nanomesh membranes for rapid water transport and precise ion/molecular sieving. The resulting SNGMs effectively address the trade-off between water permeability and ion selectivity in conventional desalination membranes, delivering a water permeability of ～ 1–2 orders of magnitude higher than that of commercial membranes, while maintaining a comparable ion rejection ratio(>95% for Na Cl). This advance marks a significant leap forward in adopting 2D nanoporous membranes for desalination technology.

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Anti-Dehydration and Stable Mechanical Properties During the Phase Transition of the Pnipam-Based Hydrogel for Body Temperature Monitoring Sensors

SSRN

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SSRN 2024年

作者： Zhang, Xiaoyong Ding, Haoran Zhou, Yujia Li, Zhaozhao Bai, Yongping Zhang, Lidong School of Materials Science and Engineering Anhui Province Key Laboratory of Specialty Polymers Anhui University of Science and Technology Anhui Huainan232001 China Department of Oil Storage and Transportation Engineering China University of Petroleum-Beijing Beijing100100 China School of Chemistry and Chemical Engineering Harbin Institute of Technology Heilongjiang Harbin150000 China School of Chemistry and Molecular Engineering East China Normal University Shanghai200241 China

Poly(N-isopropylacrylamide) (PNIPAM) enhances the reversibility and responsiveness of wearable temperature-sensitive devices. However, an open question is whether and how the hydrogel design can prevent adhesive performance loss caused by phase transition-induced dehydration and unstable mechanical properties between devices and human-skin and reduce interfacial failure. Herein, a gelatin-mesh scaffold-based hydrogel (NAGP-Gel) is constructed to inhibit dehydration and volume change, leading to stable mechanical properties, superior adhesiveness, and thermal sensing sensitivity during phase transition. The gelatin enhances the polymer chains-water interaction and weakens the degree of aggregation of polymer chains-chains, improving anti-dehydration properties under 45 oC conditions that are higher than lower critical solution temperature (LCST, i.e., ~32 °C). The mesh scaffold greatly restricts the phase-transition-induced polymer chain movement and maintains mechanical performance. In 60 oC environment, the maximum water loss and volume retention ratio of the NAGP-Gel are only 3.58 % and 97.3%, respectively. Additionally, NAGP-Gel serves as a temperature sensor producing a stable thermal-electrical signal within the LCST range. It also can be assembled into an electronic device enables the transmission of information and recognization of sign language via Morse code. This work broadens the application of PNIPAM in constructing intelligent hydrogels and opens a new door to exploring emerging hydrogels for temperature monitoring applications. © 2024, The Authors. All rights reserved.

关键词： Hydrogels

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molecular Insights into n-Type Organic Thermoelectrics

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CCS Chemistry 2021年第10期3卷 2702-2716页

作者： Shuyan Shao Jian Liu Institute of Molecular Aggregation Science Tianjin UniversityTianjin 300072 Zernike Institute of Advanced Materials University of Groningen9747 AG Groningen Department of Chemistry and Chemical Engineering Chalmers University of TechnologyGöteborg 41296

Organic thermoelectrics(OTEs)have been recently intensively investigated as they hold promise for flexible,large-area,and low-cost energy generation or heating–cooling devices for appealing applications,for example,wearable energy *** the past 7 years,n-type OTEs have witnessed a sharp increase in their performance thanks to significant progress in developing and understanding the fundamental physical properties of n-type OTE materials as well as the working principle and physical processes of the TE devices.

关键词： organic thermoelectrics n-type organic semico nductors mo lecular doping side-chain engi-neering back bone mod ifi cation

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Antitumor efficacy and potential mechanism of FAP-targeted radioligand therapy combined with immune checkpoint blockade

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Signal Transduction and Targeted Therapy 2024年第7期9卷 2936-2952页

作者： Liang Zhao Yizhen Pang Yangfan Zhou Jianhao Chen Hao Fu Wei Guo Weizhi Xu Xin Xue Guoqiang Su Long Sun Hua Wu Jingjing Zhang Zhanxiang Wang Qin Lin Xiaoyuan Chen Haojun Chen Department of Nuclear Medicine and Minnan PET Center Xiamen Key Laboratory of RadiopharmaceuticalsThe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamenChina Departments of Diagnostic Radiology SurgeryChemical and Biomolecular Engineeringand Biomedical EngineeringYong Loo Lin School of Medicine and College of Design and EngineeringNational University of SingaporeSingaporeSingapore Clinical Imaging Research Centre Centre for Translational MedicineYong Loo Lin School of MedicineNational University of SingaporeSingaporeSingapore Department of Radiation Oncology Xiamen Cancer CenterXiamen Key Laboratory of Radiation OncologyThe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamenChina Department of Colorectal Tumor Surgery Xiamen Cancer CenterXiamen Key Laboratory of Radiation OncologyThe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamenChina Department of Cardiothoracic Surgery Zhongda HospitalSchool of MedicineSoutheast UniversityNanjingChina Nanomedicine Translational Research Program NUS Center for NanomedicineYong Loo Lin School of MedicineNational University of SingaporeSingaporeSingapore Department of Neurosurgery and Department of Neuroscience Fujian Key Laboratory of Brain Tumors Diagnosis and Precision TreatmentXiamen Key Laboratory of Brain Centerthe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamenChina Institute of Molecular and Cell Biology Agency for ScienceTechnology and Research(A*STAR)SingaporeSingapore Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamenChina

Radiotherapy combined with immune checkpoint blockade holds great promise for synergistic antitumor *** radionuclide therapy delivers radiation directly to tumor ***1004 is a fibroblast activation protein(FAP)-targeting radiopharmaceutical,conjugated with the albumin binder Evans Blue,which has demonstrated enhanced tumor uptake and retention in previous preclinical and clinical ***,we demonstrate that^(68)Ga/^(177)Lu-labeled LNC1004 exhibits increased uptake and prolonged retention in MC38/NIH3T3-FAP and CT26/NIH3T3-FAP tumor *** therapy with^(177)Lu-LNC1004 induced a transient upregulation of PD-L1 expression in tumor *** combination of^(177)Lu-LNC1004 and anti-PD-L1 immunotherapy led to complete eradication of all tumors in MC38/NIH3T3-FAP tumor-bearing mice,with mice showing 100%tumor rejection upon ***,single-cell RNA sequencing(scRNA-seq),and TCR sequencing revealed that combination therapy reprogrammed the tumor microenvironment in mice to foster antitumor immunity by suppressing malignant progression and increasing cell-to-cell communication,CD8^(+)T-cell activation and expansion,M1 macrophage counts,antitumor activity of neutrophils,and T-cell receptor diversity.A preliminary clinical study demonstrated that^(177)Lu-LNC1004 was well-tolerated and effective in patients with refractory ***,scRNA-seq of peripheral blood mononuclear cells underscored the importance of addressing immune evasion through immune checkpoint blockade *** was emphasized by the observed increase in antigen processing and presentation juxtaposed with T cell *** conclusion,our data supported the efficacy of immunotherapy combined with^(177)Lu-LNC1004 for cancer patients with FAP-positive tumors.

关键词： immunity retention holds

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Study on the Modulating Effect of Halogen Atom Substitution on the Detection Range of Water Content Detection Probes in Organic Solvents

SSRN

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SSRN 2023年

作者： Wu, Qiong Xu, Jiajun Huang, Meifeng Zhang, Siman Ning, Dan Pang, Haijun Jiao, Liang Yang, Qiuling Yang, Jiao Department of Chemical Science and Technology Kunming University Yunnan Kunming650214 China College of Physics Science and Technology Kunming University Yunnan Kunming650214 China The School of Material Science and Chemical Engineering Harbin University of Science and Technology Harbin150040 China Yunnan Key Laboratory of Metal-Organic Molecular Materials and Device School of Chemistry and Chemical Engineering Kunming University Kunming650214 China

Fluorescence probes based on the variations of aggregation state (Aggregation-Induced Emission (AIE) and Aggregation-Caused Quenching (ACQ)) have received widespread attention due to their simplicity, efficiency and intuitiveness. However, typical probes are highly sensitive to changes in polarity, and slight variations in the external environment can cause a complete change in the aggregation state. With the aim of expanding the detection range of the molecular probe, this work adopts a different design strategy from adjusting the molecular backbone but regulates the fluorescence behavior of the Schiff base molecular backbone by introducing different halogen atoms. Systematic studies show that when chlorine serves as substitutional atoms (3,5-Cl Salen), the probe can achieve full-range detection of water content (0-100 wt%) in ethanol and DMF. To our knowledge, the 3,5-Cl Salen represents the best water content probe in organic molecules. Experimental and theoretical studies have shown that the adjustion of halogen atoms can linearly change the charge distribution on the benzene ring, and precisely controlling the strength of intermolecular interactions. At the same time, we developed a fluorescent filter paper based on 3,5-Cl Salen and used smartphones for rapid, sensitive and precise on-site measurement of water content in organic solvents. © 2023, The Authors. All rights reserved.

关键词： Organic solvents

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