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Valence electron matching law for MXene-based single-atom catalysts

Journal of Energy Chemistry 2025年第2期101卷 641-650页

作者： Pei Song Yuhang Zhou Zishan Luo Hang Zhang Xi Sun Sen Lu Zepeng Jia Hong Cui Weizhi Tian Rong Feng Lingxia Jin Hongkuan Yuan School of Mechanical Engineering Shaanxi University of Technology Shaanxi Key Laboratory of industrial Automation Shaanxi University of Technology Shaanxi Key Laboratory of Catalysis College of Chemical & Environment Science Shaanxi University of Technology School of physical Science and Technology Southwest University

Single-atom catalysts（SACs） have attracted considerable interest in the fields of energy and environmental science due to their adjustable catalytic *** this study,we investigated the matching of valence electron numbers between single atoms and adsorbed intermediates（O,N,C,and H） in MXene-anchored SACs（M-Ti2C/M-Ti2CO2）.The density functional theory results demonstrated that the sum of the valence electron number（VM） of the interface-doped metal and the valence electron number（VA） of the adsorbed intermediates in M-Ti2C followed the 10-valence electron matching ***,based on the 10-valence electron matching law,we deduced that the sum of the valence electron number（k） and VMfor the molecular adsorption intermediate interactions in M-Ti2CO2adhered to the 11-valence electron matching *** repulsion between the interface electrons in M-Ti2CO2and H2O weakened the adsorption of intermediates,Furthermore,we applied the 11-valence electron matching law to guide the design of catalysts for nitrogen reduction reaction,specifically for N2→ NNH conversion,in the *** sure independence screening and sparsifying operator algorithm was used to fit a simple three-dimensional descriptor of the adsorbate（R2up to 0.970） for catalyst *** study introduced a valence electron matching principle between doped metals（single atoms） and adsorbed intermediates（atomic and molecular） for MXene-based catalysts,providing new insights into the design of high-performance SACs.

关键词： Density functional theory Nitrogen reduction reaction Sure independence screening and sparsifying operator Valence electron matching law

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Development of a net ozone production rate detection system based on dual-channel cavity ring-down spectroscopy

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Journal of Environmental Sciences 2025年第3期149卷 419-430页

作者： Jinzhao Tong Renzhi Hu Changjin Hu Xiaoyan Liu Haotian Cai Chuan Lin Liujun Zhong JiaweiWang Pinhua Xie School of Environmental Science and Optoelectronic Technology University of Science and Technology of ChinaHefei 230026China Anhui Institute of Optics and Fine Mechanics Hefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China School of pharmacy Anhui Medical UniversityHefei 230032China

A novel system for measuring net photochemical ozone production rates in the atmosphere based on cavity ring-down spectroscopy(OPR-CRDS)was *** system consists of two chambers(a reaction chamber and a reference chamber)and a dual-channel O_(x)-CRDS *** minimize the wall loss of O_(x)in the chambers,the inner surfaces of both chambers are coated with Teflon *** performance of the OPR-CRDS system was *** was found that even though the photolysis frequency(J value)decreased by 10%,the decrease in the P(O_(3))caused by the ultraviolet-blocking film coating was less than 3%.The two chambers had a good consistency in the mean residence time and the measurement of NO_(2)and O_(x)under the condition of no *** detection limit of the OPR-CRDS was determined to be 0.20 ppbv/*** further verify the accuracy of the system,the direct measurement values of the OPR-CRDS systemwere comparedwith the calculation results based on radical(OH,HO_(2),and RO_(2))reactions,and a good correlation was obtained between the measured and calculated ***,the developed instrument was applied to obtain the comprehensive field observations at an urban site in the Yangtze River Delta(China)for 40 days,the time series and change characteristics of the P(O_(3))were obtained directly,and the good environmental adaptability and stability of the OPR-CRDS system were *** is expected that the new instrument will be beneficial to investigations of the relationship between P(O_(3))and its precursors.

关键词： Ozone Net photochemical production rate CRDS Atmospheric chemistry

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Enhanced oral drug delivery by mimicking natural amino acid and oligopeptide absorption route

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Nano Research 2025年第2期18卷 525-540页

作者： Ruinan Wu Xiaoxing Fan Licheng Wu Liyun Xing Jinxia Kong Zhou Zhou Jingyuan Wen Lian Li Yuan Huang Key Laboratory of Drug-Targeting and Drug Delivery System of the Education Ministry and Sichuan Province Sichuan Engineering Laboratory for Plant-Sourced Drug and Sichuan Research Center for Drug Precision Industrial TechnologyWest China School of PharmacySichuan UniversityChengdu 610041China School of pharmacy Faculty of Medical and Health SciencesUniversity of AucklandAuckland 1023New Zealand

Oral delivery of protein and peptide drugs presents considerable challenges due to their susceptibility to digestive enzymes in gastrointestinal(Gl)tract and low efficiency of transepithelial ***,inspired by efficient absorption of protein-based nutrients,we constructed several kinds of oral drug delivery systems by mimicking natural amino acid and oligopeptide absorption *** kinds of amino acids and two kinds of oligopeptides were chosen as targeting ligands to mediate transportation of orally administered nanoparticles(NPs).Liraglutide(Lira),a kind of glucagon like peptide-1(GLP-1)receptor agonist,was used as model *** functionalized NPs could protect Lira from enzymatic degradation in Gl ***,compared with amino acid-modified NPs,oligopeptide-modified NPs exhibited greater transepithelial transport efficiency and were primarily absorbed in the proximal small intestine due to the high expression and transportation mediated by proton coupled oligopeptide transporter 1(PEPT1).These Lira-loaded NPs could effectively control the blood glucose level,reduce plasma lipid level,and repair tissue damage on type 2 diabetic mice and even showed comparable hypoglycemic effects of subcutaneous injection(s.c.)free *** study demonstrates the potential of mimicking natural oligopeptide absorption route to enhance oral delivery of protein and peptide drugs.

关键词： oral drug delivery amino acid absorption route oligopeptide absorption route liraglutide

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Chiral phosphoramidite ligand-modulated palladium auto-tandem catalysis for asymmetric dehydrogenative dienylation of imines with α-alkenes

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Science China Chemistry 2025年

作者： Zhong-Sheng Nong Hao-Fan Qian Ying-Chun Chen Pu-Sheng Wang Liu-Zhu Gong Hefei National Research Center for physical Sciences at the Microscale and Department of Chemistry University of Science and Technology of China Key Laboratory of Drug Targeting and Drug Delivery System (Sichuan University) Ministry of Education and Sichuan Research Center for Drug Precision Industrial Technology West China School of Pharmacy Sichuan University School of Materials and Chemistry Southwest University of Science and Technology

The development of efficient processes allowing rapid access to complex chiral molecules from easily available alkenes is a long-term pursuit in the synthetic chemistry community. Transition metal-catalyzed asymmetric functionalization of allylic C–H bond represents a unique alternative toward this goal. However, enantioselective dehydrogenative transformation of olefins to value-added optically enriched molecules remains yet to be discovered. Here, we report a highly enantioselective dehydrogenative dienylation of imines with unactivated α-alkenes driven by the synergistic action of palladium complex and carboxylic acid. Chiral phosphoramidite ligands turned out to be superior in modulating the performance of palladium autotandem catalysis and allowed a broad range of α-alkenes and imines to be transformed into chiral dienylamines. Mechanistic studies suggest that the dienes could be in situ generated from α-alkenes through a palladium(0)-mediated dehydrogenative process in the presence of excess benzoquinone oxidants, and then participated in the Pd-chiral phosphoramidite-catalyzed intermolecular vinylogous-type addition to the imines activated by the carboxylic acid co-catalyst. Notably, the second β-H elimination occurring in the dienylation event might be the turnover-limiting step.

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Oscillatory flow reactor facilitates fast photochemical Wolff rearrangement toward synthesis of α-substituted amides in flow

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Chinese Chemical Letters 2025年第2期36卷 389-393页

作者： Huashan Huang Jingze Chen Luyun Zhang Hong Yan Siqi Li Fen-Er Chen Institute of Pharmaceutical Science and Technology College of Chemistry Fuzhou University Key Laboratory of Natural Medicines of the Changbai Mountain Ministry of Education Molecular Medicine Research Center College of Pharmacy Yanbian University Engineering Center of Catalysis and Synthesis for Chiral Molecules Department of Chemistry Fudan University Shanghai Engineering Center of industrial Catalysis for Chiral Drugs

A visible light-promoted fast photochemical Wolff rearrangement was developed toward synthesis of α-substituted amides in continuous flow with the use of a photochemical oscillatory flow reactor(POFR).The control experiment indicates that a fast process of the Wolff rearrangement(<40 s) is involved. Notably, this protocol does not require excess use of any reactants, and the resulting α-substituted amides could be isolated by recrystallization in good to excellent yields.

关键词： Flow photochemistry Ketene Oscillatory flow reactor Wolff rearrangement α-Substituted amides

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Tandem asymmetric dearomatized functionalization reaction of phenols with Evans-ynamides enabled by divergent electrophiles

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Science China Chemistry 2025年第2期68卷 649-660页

作者： Ying-Qi Zhang Gan-Lu Qian Yun Liu Jia-Hui Li Xin Hong Zhou Xu Bo Zhou Long-Wu Ye State Key Laboratory of physical Chemistry of Solid Surfaces Key Laboratory of Chemical Biology of Fujian Provinceand College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Center of Chemistry for Frontier Technologies Department of ChemistryState Key Laboratory of Clean Energy UtilizationZhejiang UniversityHangzhou 310027China Jiangsu Key Laboratory of New Drug Research and Clinical pharmacy School of PharmacyXuzhou Medical UniversityXuzhou 221004China State Key Laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 300071China State Key Laboratory of Organometallic Chemistry Chinese Academy of SciencesShanghai 200032China

Herein,we disclose a highly regio-/chemoselective tandem asymmetric dearomatized halofunctionalization reaction of phenoltethered ynamides with diverse electrophilic halogenation sources in a catalyst-free manner for the practical and rapid assembly of a series of halogenated spirocyclic ***,the related dearomatized selenation and protonation are also achieved,affording the corresponding selenated and protonated spirocycles in high ***,the enantioselectivities of these products can be perfectly induced by Evans auxiliaries(99%ees).Significantly,this protocol not only represents the first tandem asymmetric halofunctionalization reaction of phenol derivatives,but also constitutes the first asymmetric halogenation/selenation of *** calculations indicate a remote induction model of Evans chiral auxiliary-attached keteniminium.

关键词： alkynes cyclization dearomatization Evans chiral auxiliary spirocycles

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physical Layer Security Scheme With AoI-Awareness for industrial IoT Based on Covert Communications

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IEEE/CAA Journal of Automatica Sinica 2025年第1期12卷 276-278页

作者： Yaping Li Zhi-Xin Liu Jia-Wei Su Ya-Zhou Yuan the Key Laboratory of industrial Computer Control Engineering of Hebei Province Yanshan University

Dear Editor,industrial Internet of things(IIoT) is a typical application of cyberphysical system(CPS). In the IIoT, wireless communication is an inevitable trend to replace the deployment-limited wired transmission for cases with large-scale and mobile devices. However, wireless communication gives rise to critical issues related to physical security, such as malicious detections and attacks [1].

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Spatial-temporal distribution and emission of urban scale air pollutants in Hefei based on Mobile-DOAS

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Journal of Environmental Sciences 2025年第5期151卷 238-251页

作者： Zhidong Zhang Pinhua Xie Ang Li Min Qin Jin Xu Zhaokun Hu Xin Tian Feng Hu Yinsheng Lv Jiangyi Zheng Youtao Li School of Environmental Science and Optoelectronic Technology University of Science and Technology of ChinaHefei 230026China Key Laboratory of Environmental Optics and Technology Anhui Institute of Optics and Fine MechanicsHefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China University of Chinese Academy of Sciences Beijing 100049China Information Materials and Intelligent Sensing Laboratory of Anhui Province Institutes of Physical Science and Information TechnologyAnhui UniversityHefei 230601China

As a significant city in the Yangtze River Delta regions,Hefei has experienced rapid changes in the sources of air pollution due to its high-speed economic development and urban ***,there has been limited research in recent years on the spatial-temporal distribution and emission of its atmospheric *** address this,this study conducted mobile observations of urban roads using the Mobile-DOAS instrument from June 2021 to May *** monitoring results exhibit a favourable consistent with TROPOMI satellite data and ground monitoring station ***,there were pronounced seasonal variations in air ***,high concentration of HCHO and NO_(2)were closely associated with traffic congestion on roadways,while heightened SO_(2)levels were attributed to winter heating and industrial *** study also revealed that with the implementation of road policies,the average vehicle speed increased by 95.4%,while the NO concentration decreased by 54.4%.In the estimation of urban NO_(x)emission flux,it was observed that in temporal terms,compared with inventory data,the emissions calculated viamobile measurements exhibitedmore distinct seasonal patterns,with the highest emission rate of 349 g/sec in winter and the lowest of 142 g/sec in *** spatial terms,the significant difference in emissions between the inner and outer ring roads also suggests the presence of the city’s primary NO_(x)emission sources in the area between these two *** study offers data support for formulating the next phase of air pollution control measures in urban areas.

关键词： Mobile-DOAS HCHO NO_(2) SO_(2) Spatial-temporal distribution NOx emission

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An Evaluation on physical Characteristics of Konjac Polysaccharides-Based Film Coating and Its Application for Strawberries Preservation

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Journal of Renewable Materials 2025年第1期13卷 181-197页

作者： Desy Nurliasari Awaly Ilham Dewantoro Muhammad Adly Rahandi Lubis Roni Kastaman Mohamad Djali Efri Mardawati Devi Maulida Rahmah Siti Nurhasanah Akbar Hanif Dawam Abdullah Lukmanul Hakim Zaini Department of Agricultural industrial Technology Faculty of Agro-Industrial TechnologyUniversitas PadjadjaranJatinangor45363Indonesia Research Center for Biomass and Bioproducts National and Innovation AgencyCibinong1691Indonesia Research Collaboration Center for Biomass and Biorefinery between BRIN and Universitas Padjadjaran Jatinangor45363Indonesia Research Center for Appropriate Technology Universitas PadjadjaranJatinangor45363Indonesia Department of Food industrial Technology Faculty of Agro-Industrial TechnologyUniversitas PadjadjaranJatinangor45363Indonesia Department of Forest Products Faculty of Forestry and EnvironmentIPB UniversityBogor16680Indonesia Institute of Wood Technology and Renewable Materials Department of Material Sciences and Process EngineeringUniversity of Natural Resources and Life SciencesVienna(BOKU)Vienna1180Austria

Konjac is an ideal candidate for edible coatings on fruits due to its hydrophilic properties,ﬁlm-forming ability,barrier properties,safety,and ***,the high market demand for strawberries necessitates post-harvest treatment to extend their shelf life and preserve their quality,as strawberries are known for their fragile skin and soft *** fully utilize konjac and develop high-quality coatingﬁlms,native konjacﬂour(NKF)and konjac glucomannan(KGM)were extracted from its corm and used as a coatingﬁlm for strawberries in the present ***,this study aimed to compare the physical properties of theﬁlm coatings between NKF and KGM,and evaluate their effects on strawberries preservation over 7 days of storage.A multistage extrac-tion process was employed to isolate NKF and KGM,after which the glucomannan content was *** yield was 31.81%,exceeding KGM yield of 26.42%,and the glucomannan content obtained of NKF(25.93%)was higher than KGM(21.41%).Nuclear magnetic resonance spectroscopy conﬁrmed that both NKF and KGM con-tain glucomannan in their ***,both NKF and KGM were combined with carboxymethyl cel-lulose(CMC)and glycerol to produce eight thin-layerﬁlms to assess their physical and mechanical *** to the KGM variant,the NKF variant generally exhibited higher moisture content,water vapor trans-mission rate,and tensile ***,NKF was less effective than KGM in extending strawberry storage life,leading to faster color changes and greater weight loss,despite maintaining similar hardness ***,konjac-based coatings were generally effective at maintaining the freshness and quality of strawberries compared to uncoated *** shows promise as an edible coating,improving fresh produce shelf life and appeal,aligning with consumer preferences for natural and sustainable products.

关键词： Amorphophalus oncophyllus coating performances edibleﬁlm strawberry preservation

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Pharmaceutical amorphous solid dispersion: A review of manufacturing strategies

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Acta Pharmaceutica Sinica B 2021年第8期11卷 2505-2536页

作者： Sonal V.Bhujbal Biplob Mitra Uday Jain Yuchuan Gong Anjali Agrawal Shyam Karki Lynne S.Taylor Sumit Kumar Qi(Tony)Zhou Department of industrial and physical pharmacy College of PharmacyPurdue University Oral Product Development Bristol Myers Squibb Material Science and Engineering Bristol Myers Squibb

Amorphous solid dispersions(ASDs)are popular for enhancing the solubility and bioavailability of poorly water-soluble *** approaches have been employed to produce ASDs and novel techniques are *** review provides an updated overview of manufacturing techniques for preparing *** physical stability is a critical quality attribute for ASD,the impact of formulation,equipment,and process variables,together with the downstream processing on physical stability of ASDs have been *** strategies are proposed to identify suitable manufacturing methods,which may aid in the development of ASDs with satisfactory physical stability.

关键词： Amorphous solid dispersions Stability Drug delivery Manufacturing Solvent evaporation Melting process Co-precipitation Downstream processing Selection criteria

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