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Rapid Synthesis of Ultrafine Ru Nanoparticles Anchoring Onto Tungsten Carbide with Strong Synergetic Interaction as Highly Efficient Hydrogen Evolution Reaction Electrocatalyst

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SSRN 2023年

作者： Zong, Lingbo Wang, Chengbin Li, Ping Fan, Kaicai Lu, Fenghong Wang, Zumin Wang, Lei Key Laboratory of Eco-chemical Engineering College of Chemistry and Molecular Engineering Qingdao University of Science and Technology Qingdao266042 China College of Materials Science and Engineering Qingdao University of Science and Technology Qingdao266042 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences 1 North 2nd Street Zhongguancun Haidian District Beijing100190 China Chaofeng Steel Structure Group Co. Ltd. Xiaoshan Economic and Technological Development Zone No. 38 Beitang Road Zhejiang Hangzhou China

Developing cost effective, active and durable alternatives to platinum electrocatalysts is the major challenge for sustainable hydrogen production. Rational design and controlled synthesis of hybrid structures with tunable metal-support interaction may offer a feasible strategy to achieve efficient and stable hydrogen evolution reaction (HER). Herein, a low cost and high-performance Ru/WC HER electrocatalyst was successfully prepared by flash joule heating technology, which can be accomplished in less than 1.0 second. Through this method, ultrasmall Ru nanoparticles (~2 nm) were uniformly dispersed on the simultaneously generated WC support with intimate contact and strong electronic interactions. Because of the synergetic effects, the electron transfer between Ru and WC significantly improved, and the active sites exposed largely increased. In a strong alkaline medium, the as-prepared Ru/WC exhibits a low overpotential of 4 mV and 72 mV at current densities of 10 mA cm−2 and 100 mA cm−2, respectively. The low Tafel slope of 44 mV dec−1 and a slight shift in overpotential after 5000 CV cycles demonstrated the fast kinetics and high stability of Ru/WC, which was much better than the benchmark Pt/C. Furthermore, Ru/WC also showed excellent activity under acidic conditions and maintained its original properties for 5000 CV cycles. Notably, Ru/WC can accommodate HER current density as high as 2000 mA cm−2 with small overpotentials (365 mV), which hold great promises for industrial large-scale production. This work provides a simple and rapid strategy for synthesizing high efficiency HER catalyst. © 2023, The Authors. All rights reserved.

关键词： Electrocatalysts

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Snowball Flower-Like G-C3n4/Znfe2o4 Mesoporous Hollow Microspheres with Enhanced Triethylamine Sensing Properties

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SSRN 2022年

作者： Wang, Hong Fu, Yuehao Liu, Xiaohua Yang, Ruisong Hu, Yu Liu, Di Wan, Jiawei Zeng, Zhipeng School of Materials Science and Engineering Sichuan University of Science & Engineering Zigong643000 China Material Corrosion and Protection Key Laboratory of Sichuan Province Sichuan University of Science & Engineering Zigong643000 China Department of Chemistry Tsinghua University Beijing100084 China State Key Laboratory of Biochemical Engineering CAS Center for Excellence in Nanoscience Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China

Herein, the snowball flower-like g-C3N4/ZnFe2O4 mesoporous hollow microspheres, in which two-dimensional (2D) g-C3N4 nanolayers were loaded onto the surface of ZnFe2O4 hollow microsp... 详细信息

Herein, the snowball flower-like g-C3N4/ZnFe2O4 mesoporous hollow microspheres, in which two-dimensional (2D) g-C3N4 nanolayers were loaded onto the surface of ZnFe2O4 hollow microspheres, were constructed by a simple solid phase reaction. The effect of the g-C3N4 concentration on the structure, morphology and gas-sensing performance of the g-C3N4/ZnFe2O4 composites had been explored. On the basis of gas sensitivity test results, the composites owned lower working temperature (160 ℃) and better selectivity toward TEA in comparison with pure ZnFe2O4. Notably, the sensor based on the g-C3N4/ZnFe2O4-15 hollow microspheres (adding 15ml of g-C3N4 aqueous solution) exhibited outstanding sensing properties, including superior response (18.3) toward 100 ppm TEA at optimum work temperature of 160 ℃, speedy response-recovery time (33, 30 s) and outstanding stability. And the sensor maintained high response of 4.3 to low concentration TEA (5 ppm). The improved gas-sensing performance of the composites could be attributed to the porous ZnFe2O4 hollow microspheres loaded by 2D g-C3N4 nanolayers with large specific surface area and the heterostructure formed between them. Hence, a potential application of the g-C3N4/ZnFe2O4 microspheres might be achieved in detecting TEA at a low optimum work temperature. © 2022, The Authors. All rights reserved.

关键词： Zinc compounds

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Griffithazanone A, a sensitizer of EGFR-targeted drug in Goniothalamus yunnanensis for non-small cell lung cancer

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Heliyon 2024年第19期10卷 e38489页

作者： Xiao, Ting Zhu, Yuxin Zhang, Liang Xiao, Kaidi Jia, Xiao Liu, Yashu Bi, Junfang Li, Xiaoping Zhou, Honggang Yang, Cheng State Key Laboratory of Separation Membranes and Membrane Processes Tianjin Key Laboratory of Green Chemical Technology and Process Engineering School of Pharmaceutical Sciences Tiangong University Tianjin 300387 China State Key Laboratory of Medicinal Biology College of Pharmacy and Tianjin Key Laboratory of Molecular Drug Research Department of Thoracic Surgery Tianjin First Central Hospital Nankai University Haihe Education Park 38 Tongyan Road Tianjin 300353 China Tianjin Key Laboratory of Molecular Drug Research Tianjin International Joint Academy of Biomedicine Tianjin 300457 China Department of Combined Traditional Chinese Medicine and West Medicine Traditional Chinese Medicine Hospital of Shijiazhuang City Shijiazhuang 050051 China

Non-small cell lung cancer (NSCLC), which accounts for up to 85 % of lung cancer cases, significantly impacts the health of individuals worldwide. While targeted therapy has played a crucial role, the emergence of EGFR resistance and adverse reactions has made it imperative to explore new medications. Natural products derived from plants became an important source of anti-tumor drugs. In this study, nine known compounds, including seven alkaloids (1–7) and two styryllactones (8 and 9) were isolated from twigs and leaves of Goniothalamus yunnanensis. Their structures were elucidated by their NMR spectroscopic data. Among them, griffithazanone A (1) showed the strongest inhibitory activity with the IC₅₀ value of 6.775 μM. Our findings revealed that griffithazanone A treatment induced cytotoxicity, apoptosis, and ROS generation in A549 cells in a dose-dependent manner. It regulates the expression of apoptosis-related proteins Bax, Bcl-2, and cleaved-caspase3 both in vitro and in vivo. Further investigation demonstrated that griffithazanone A regulated the proteins involved in the ASK1/JNK/p38 and BAD/Bcl-2 pathways in A549 cells by targeting PIM1. Moreover, griffithazanone A treatment enhanced the efficacy of gefitinib and osimertinib and reversed osimertinib resistance. Overall, our study highlights the potential of griffithazanone A in inhibiting the progression of NSCLC by targeting PIM1 and reversing resistance to EGFR targeted drugs. © 2024

关键词： Apoptosis Griffithazanone A Osimertinib resistant PIM1

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An effective strategy for degrading waste PET plastic into regenerated DMT with nearly equivalent methanol at relatively low temperature

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Chemical engineering Science 2025年 315卷

作者： Rong, Chunrui Yan, Dongxia Li, Jiabao Feng, Jian Xin, Jiayu Zhou, Qing Li, Yi Xu, Junli Lu, Xingmei Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Sino Danish College University of Chinese Academy of Sciences Beijing100049 China School of Chemical and Engineering University of Chinese Academy of Sciences Beijing100049 China Key Laboratory for Green Process of Chemical Engineering of Xinjiang Bingtuan School of Chemistry and Chemical Engineering Shihezi University Shihezi832003 China

The increase in the usage of polyethylene terephthalate (PET) leads to the generation of a large amount of waste, which may cause carbon emissions and waste of petroleum resources. The methanolysis method has attracted global attention, but limited by high reaction temperature and excessive use of methanol. We report here an efficient catalyst, tetramethylguanidine/1,5-diazabicyclo[4.3.0]-5-non-ene (TMG/DBN), converting waste PET into regenerated dimethyl terephthalate (rDMT) under 100 °C with almost equivalent methanol, achieving 100 % PET conversion and 93.1 % yield of rDMT. A series of analytical methods and theoretical calculations were used to reveal the enhanced interaction between the catalyst and reactants, which facilitates the degradation of PET at low methanol dosages. In addition, a kinetic model was also developed with a relatively low activation energy of 84.9 kJ/mol. This work provides an effective strategy for the up-grading recycling of waste PET under mild reaction conditions. © 2025

关键词： Petroleum deposits

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Fabrication of high-capacity cation-exchangers for protein adsorption: Comparison of grafting-from and grafting-to approaches

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Frontiers of Chemical Science and engineering 2019年第1期13卷 120-132页

作者： Ming Zhao Run Liu Jian Luo Yan Sun Qinghong Shi Department of Biochemical Engineering School of Chemical Engineering and Technology Tianjin University Tianjin 300350 China Key Laboratory of Systems Bioengineering (Ministry of Education) Tianjin University Tianjin 300072 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China

In this work, we have synthesized two polymer-grafted cation exchangers: one via the grafting-from approach, in which sulfopropyl methacrylate (SPM) is grafted through atom transfer radical polymerization onto Sepharose FF (the thus resulting exchanger is referred as Sep-g-SPM), and another via the grafting-to approach, in which the polymer of SPM is directly coupled onto Sepharose FF (the thus resulting exchanger is called as Sep-pSPM). Protein adsorption on these two cation exchangers have been also investigated. At the same ligand density, Sep-g-SPM has a larger accessible pore radius and a smaller depth of polymer layer than Sep-pSPM, due to the controllable introduction of polymer chains with the regular distribution of the ligand. Therefore, high-capacity adsorption of lysozyme and γ-globulin could be achieved simultaneously in Sep-g-SPM with an ionic capacity (IC) of 308 mmol·L^-1. However, Sep-pSPM has an irregular chain distribution and different architecture of polymer layer, which lead to more serious repulsive interaction to proteins, and thus Sep-pSPM has a lower adsorption capacity for γ-globulin than Sep-g-SPM with the similar IC. Moreover, the results from protein uptake experiments indicate that the facilitated transport of adsorbed γ-globulin occurs only in Sep-pSPM and depends on the architecture of polymer layers. Our research provides a clear clue for the development of high-performance protein chromatography.

关键词： polymer-grafted ionic exchanger grafting technique protein adsorption atom transfer radical polymerization γ-globulin

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Steering Phase-Separated Droplets to Control Fibrillar Network Evolution of Supramolecular Peptide Hydrogels

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SSRN 2022年

作者： Zhou, Peng Xing, Ruirui Li, Qi Li, Junbai Yuan, Chengqian Yan, Xuehai State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Beijing National Laboratory for Molecular Sciences CAS Key Lab of Colloid Interface and Chemical Thermodynamics Institute of Chemistry Chinese Academy of Sciences Beijing100190 China University of Chinese Academy of Sciences Beijing100049 China Center for Mesoscience Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China

Controlling the non-covalent cross-linking network morphology of supramolecular hydrogels is of primary importance in tuning their mechanical properties for practical biomaterial applications. In this work, we study the fibrillar network evolution that controls the mechanical properties of the hydrogels by modulating the solute-rich metastable droplets formed via liquid liquid phase separation (LLPS). The size and amount of the droplets, the structural evolution of droplets into pre-fibrils, and fibril network development can be finely tuned by varying the thermal history. There is an optimal initial incubation temperature leading to the hydrogel with the optimized mechanical strength and recovery performance. The mechanism of the temperature dependence of mechanical properties is due to the different non-covalent cross linked gel network morphology through distinct self-assembly pathways. The findings elucidate the key role of phase-separated droplets in the evolution of self-assembling networks during gelation and provide a deeper understanding of engineering supramolecular hydrogels with flexibly tunable mechanical properties. © 2022, The Authors. All rights reserved.

关键词： Molecular dynamics

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Straightforward Sulfonamidation via Metabisulfite-Mediated CrossCoupling of Nitroarenes and Boronic Acids under Transition-Metal-Free Conditionst

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Chinese Journal of Chemistry 2020年第12期38卷 1521-1525页

作者： Yaping Li Ming Wang Xuefeng Jiang Shanghai Key Laboratory of Green Chemistry and Chemical Process School of Chemistry and Molecular EngineeringEast China Norm al University3663 North Zhongshan RoadShanghai 200062China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of Sciences345 Lingling RoadShanghai 200032China

of main observation and conclusion A straightforward multicomponent sufonamidation of nitroarenes,sodium metabisulfite and boronicacids was established under transition-mnetal-free conditions to access diverse sulfonamides from readily avilable and low-cost materials *** salt sodium metabisulfite not only served as a sulfur dioxide source,but also played a key role for both activator and reductant ***,naturlly occuring biomolecules and pharmaceuticals with multiple heteroatorms and sensitive functional groups were intensivly investigated in this transformtion providing versatile sulionamides collectively,further mechanistic studies demonstrated that nitrosoarene is thekey intermediate,and the activation of boronic acid is the rate-determining step in the transformation.

关键词： boron Transition straight

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The Effect of Ligand and Acid Promoter on Hydroesterification of Ethylene to Methyl Propionate and Kinetic Studies

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SSRN 2022年

作者： Wang, Luming Li, Zengxi Wang, Erqiang Li, Chunshan School of Chemical Sciences University of Chinese Academy of Sciences Beijing100049 China Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems The National Key Laboratory of Clean and Efficient Coking Technology Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Huizhou Institute of Green Energy and Advanced Materials Advanced Energy Science and Technology Guangdong Laboratory Guangdong516081 China

A palladium/tris(4-fluorophenyl)phosphine/p -toluenesulfonic acid catalytic new system was developed for the synthesis of methyl propionate from ethylene hydroesterification. The influence mechanism of phosphine ligands and acid promoters on catalytic activity was systematically studied. A volcano relationship between the catalytic activity and the electric effect of phosphine ligand was achieved through the characterization of 31P NMR of selenium phosphine compounds. An acid strength range favourable to the hydroesterification of ethylene was found by characterizing the pKa value of Brønsted acid. Then, the effect of phosphine ligand/Pd(OAc)2 ratio, p-toluenesulfonic/Pd(OAc)2 ratio, temperature, time, and pressure on this reaction were investigated. Finally, the elementary reaction-based kinetic model was developed, which indicated the insertion of methanol into Pd-acyl species with activation barrier of 83.1 kJ/mol is the rate-determining step. © 2022, The Authors. All rights reserved.

关键词： Ethylene

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Sequence-dependent catalysis and assembly to form peptide/Au nanoenzyme for glucose and plasma GSH detecting in cancer patients

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Supramolecular Materials 2023年第1期2卷 100040-100040页

作者： Wang, Shengtao Wang, Anhe Li, Jingtao Han, Qingquan Jing, Yafeng Li, Jieling Du, Shiyu Seeberger, Peter H. Yin, Jian Bai, Shuo State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of Sciences Beijing 100190 China Key Laboratory of Carbohydrate Chemistry and Biotechnology Ministry of Education School of Biotechnology Jiangnan University Wuxi 214122 China Department of Gastroenterology China-Japan Friendship Hospital Beijing 100029 China Department of Biomolecular Systems Max Planck Institute of Colloids and Interfaces Am Mühlenberg 1 Potsdam 14476 Germany

Metal ions play a pivotal role in regulating and determining the functions of proteins and peptides in nature. This study aims to investigate the regulatory role of metal ions in peptide assembly and explore the influence of sequence variations and metal ions on the structure and function of resulting peptide nanoarchitectures. Dipeptide sequences with distinct charged properties (positive and negative) and functional groups (-COOH, -NH₂, and phenolic hydroxyl) were meticulously selected and co-assembled with various metal ions (Au³⁺, Ag⁺, and Pt⁴⁺). The findings highlight the crucial functional role of the phenolic hydroxyl group of tyrosine in metal ion reduction, while positively charged groups promote metal ion accumulation through electrostatic forces, facilitating co-assembly. The formation of ordered structures in Au@Fmoc-YK and Au@Fmoc-YR nanoarchitectures further validates the significant interaction among metal ions, tyrosine-OH, and positively charged NH₂. Notably, these nanoarchitectures possess the unique attribute of being prepared under physiological conditions, specifically at 37 °C, without the need for organic solvents or chemical modifications of peptides. This approach offers a straightforward means of constructing diverse functional nanoarchitectures based on peptides and metal ions. Moreover, Au@Fmoc-YR exhibits good performance as a nanoenzyme for detecting glucose in complex bodily fluids and plasma GSH in tumor patients, showcasing its promising potential for medical applications. © 2023 The Authors

关键词： Biocatalysis Glucose detecting Metal ions Peptide Self-assembly Spontaneously

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Erratum on “12-tungstophosphoric acid niched in Zr-BTC: a stable and efficient catalyst for Friedel-Crafts acylation” [*** Chem., 2018, 61: 402–411]

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Science China Chemistry 2021年第8期64卷 1434-1434页

作者： Latif Ullah Guoying Zhao Zichen Xu Hongyan He Muhammad Usman Suojiang Zhang Beijing Key Laboratory of Ionic Liquids Clean Process Key Laboratory of Green Process EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences Beijing100049China Center of Excellence in Nanotechnology King Fahd University of Petroleum and MineralsDhahran3126Saudi Arabia

Erratum to:Sci China Chem,2018,61:402-411,https://***/10.1007/sll426-017-9182-0 For the above referenced publication[1],there is a correction in the Figure *** 9 Catalytic activity of pristine Zr-BTC(a),18.6 wt%HPW@Zr... 详细信息

关键词： Figure catalyst correction

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