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Pd@Ir-LOD multienzyme utilizing endogenous lactate consumption cooperates with photothermal for tumor therapy

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Nano Research 2024年第1期17卷 270-281页

作者： Zichen Ye Yun Li Jingchao Li xinyan Hu Jinyang Zheng Gongxin Zhang Sijin Xiang Tianbao Zhu Zhide Guo Xiaolan chen State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials and Engineering Research Center for Nano-Preparation Technology of Fujian ProvinceCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Molecular Vaccinology and Molecular Diagnostics&Center for Molecular Imaging and Translational Medicine School of Public Health Xiamen UniversityXiamen 361102China The High Educational Key Laboratory for Biomedical Engineering&Key Laboratory of Fire Retardant Materials of Fujian Province Department of BiomaterialsCollege of MaterialsXiamen UniversityXiamen 361102China

Lactic acid(LA)plays a major role in the occurrence,development,and spread of cancer.Enlightened by its high accumulation in tumor site,a novel lactate oxidase(LOD)conjugated two-dimensional Pd@Ir nanoplatform(Pd@Ir-LOD,PIL)was fabricated to combine cascade reaction with photothermal for tumor therapy.In detail,the overexpressed LA in tumor microenvironment(TME)was a key factor to activate the PIL-based cascade reaction:(1)Plenty of H_(2)O_(2)could be generated from LA by the catalysis of LOD with O_(2);(2)potent·OH was produced from H_(2)O_(2)due to the peroxidase(POD)-like activity of PIL;(3)meantime,PIL’s catalase(CAT)-like activity could decompose part H_(2)O_(2)into O_(2)to achieve the purpose of LA cyclic oxidization.Moreover,the reduced glutathione(GSH)scavenging capability of PIL might protect the produced reactive oxygen species(ROS)from being cleared to further improve the cascade therapeutic effect.More importantly,PIL had excellent photothermal conversion efficiency(37.35%)and manifested a surprising temperature rising effect in tumor.Taken together,the decreasing LA concentration,accumulation of high-toxic ROS,the depletion of GSH together with the higher intra-tumoral temperature potently enhanced in vivo antitumor therapy.Therefore,a promising therapeutic tactic based on PIL integrating endogenous LA consumption,chemodynamic therapy(CDT),and photothermal therapy(PTT)has been put forward.

关键词： lactate oxidase chemodynamic therapy photothermal therapy cascade reaction tumor microenvironment

Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 306-314页

作者： Yugang Qi Qing Liang Kexin Song xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun chen Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science & Engineering Electron Microscopy Center and International Center of Future Science Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials Jilin University Institute of High Energy Physics Chinese Academy of Sciences

Atom-level modulation of the coordination environment for single-atom catalysts(SACs) is considered as an effective strategy for elevating the catalytic performance. For the MNxsite, breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way, but it remains challenging for elucidating the underlying mechanism of interaction. Herein, a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks. X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR) activity as well as zinc-air battery performance. The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of *OOH, resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier, responsible for the increased intrinsic activity. Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Shell coordination optimization Single atom catalyst

Separation of chitin from shrimp shells enabled by transition metal salt aqueous solution and ionic liquid

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Chinese Journal of Chemical Engineering 2023年第1期53卷 133-141页

作者： Mi Feng Bin He xinyan chen Junli Xu Xingmei Lu Cai Jia Jian Sun Key Laboratory of Molecular Medicine and Biotherapy Ministry of Industry and Information TechnologySchool of Life SciencesBeijing Institute of TechnologyBeijing 100081China Key Laboratory of Medical Molecule Science and Pharmaceutics Engineering Ministry of Industry and Information TechnologyAdvanced Research Institute of Multidisciplinary ScienceBeijing Institute of TechnologyBeijing 100081China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex SystemsState Key Laboratory of Biochemical EngineeringBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical and Engineering University of Chinese Academy of SciencesBeijing 100049China Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing 100190China

Chitin is a widely used important industrial polymer mainly from shrimp shells, but its commercial preparation is under the great challenge of serious pollution due to the requirement of HCl and Na OH.Herein, we demonstrated that high purity chitin can be obtained from waste shrimp shells(WSSs) by cascade separation with transition metal salt aqueous solution and ionic liquid(IL). Firstly, calcium carbonate of WSSs was effectively removed in the metal salt aqueous solution driven by the ion exchange interaction. Subsequently, 1-butyl-3-methylimidazolium chloride([Bmim]Cl) had bifunctional abilities to remove residual protein and introduced metal salts simultaneously by hydrogen bonding and coordination interactions. The key experimental factors affecting the separation process were systematically studied, including the type of metal salts, temperature, and [Bmim]Cl loading. After sequential treatment with a 20%(mass) Ni SO4aqueous solution at 130 ℃ and [Bmim]Cl at 150 ℃, the purity of a-chitin can be up to 96.5%(mass) that meets commercial requirements. The use of metal salts with higher coordination ability makes the preparation of chitin no longer depend on the commonly acid-base reaction, which is conducive to the preservation of chitin structure.

关键词： Chitin Ionic liquids Transition metal salts Separation Sustainability

A post-modification strategy to precisely construct dual-atom sites for oxygen reduction electrocatalysis

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Journal of Energy Chemistry 2024年第3期90卷 511-517,I0012页

作者： Juan Wang xinyan Liu Chang-Xin Zhao Yun-Wei Song Jia-Ning Liu Xi-Yao Li chen-Xi Bi Xin Wan Jianglan Shui Hong-Jie Peng Bo-Quan Li Jia-Qi Huang School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina School of Materials Science and Engineering Beihang UniversityBeijing 100191China

Dual-atom catalysts(DACs) afford promising potential for oxygen reduction electrocatalysis due to their high atomic efficiency and high intrinsic activity.However,precise construction of dual-atom sites remains a challenge.In this work,a post-modification strategy is proposed to precisely fabricate DACs for oxygen reduction electrocatalysis.Concretely,a secondary metal precursor is introduced to the primary single-atom sites to introduce direct metal-metal interaction,which ensures the formation of desired atom pair structure during the subsequent pyrolysis process and allows for successful construction of DACs.The as-prepared FeCo-NC DAC exhibits superior oxygen reduction electrocatalytic activity with a half-wave potential of 0,91 V vs.reversible hydrogen electrode.Zn-air batteries equipped with the FeCo-NC DAC demonstrate higher peak power density than those with the Pt/C benchmark.More importantly,this post-modification strategy is demonstrated universal to achieve a variety of dual-atom sites.This work presents an effective synthesis methodology for precise construction of catalytic materials and propels their applications in energy-related devices.

关键词： Dual-atom catalysts Electrocatalysis Oxygen reduction reaction Post-modification Zinc–air batteries

Multidimensional(0D-3D)functional nanocarbon:Promising material to strengthen the photocatalytic activity of graphitic carbon nitride

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Green Energy & Environment 2021年第6期6卷 823-845页

作者： Bin He Mi Feng xinyan chen Jian Sun School of Life Science Beijing Institute of TechnologyBeijing100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing100081China

As a prospective visible-light-responsive photochemical material,graphitic carbon nitride(g-C_(3)N_(4))has become a burgeoning research hot topics and aroused a wide interest as a metal-free semiconductor in the area of energy utilization and conversion,environmental protection due to its unique properties,such as facile synthesis,high physicochemical stability,excellent electronic band structure,and sustainability.However,the shortcomings of high recombination rate of charge carriers,relatively low electrical conductivity and visible light absorption impede its practical application.Various strategies,such as surface photosensitization,heteroatom deposition,semiconductor hybridization,etc.,have been applied to overcome the barriers.Among all the strategies,functional nanocarbon materials with various dimensions(0D~3D)attract much attention as modifiers of g-C_(3)N_(4)due to their unique electronic properties,optical properties,and easy functionalization.More importantly,the properties of these functional nanocarbon materials can be tuned by various dimensions and thus there will be a way to overcome the defects of g-C_(3)N_(4)by choosing different dimensional carbon materials.Distinguishing from some present reviews,this review starts with the fundamental physicochemical characteristics of g-C_(3)N_(4)materials,followed by analyzing the advantages of functional nanocarbon materials modifying gC_(3)N_(4).Then,we present a systematic introduction to various dimensional carbon materials.The design philosophy of carbon/g-C_(3)N_(4)composites and the advanced studies are exemplified in detail.Finally,a nichetargeting summary and outlook on the major challenges,opportunities for future research in high-powered carbon/g-C_(3)N_(4)composites was proposed.

关键词： Graphitic carbon nitride(g-C_(3)N_(4)) Carbon materials Multidimension Photocatalysis Visible light

农地确权与农户政治信任:基于中央和基层组织的分析

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华中农业大学学报（社会科学版） 2024年第1期 164-177页

作者：陈卓胡新艳陈相泼湖南农业大学经济学院湖南长沙410125 华南农业大学国家农业制度与发展研究院广东广州510642

农地确权的经济影响效应受到了学界的广泛关注,但鲜有研究关注农地确权政策的政治效应。基于3期农地确权追踪调查数据,利用广义DID模型评估农地确权对农户政治信任水平的影响。结果表明:农地确权使农户的中央级政治信任、村级政治信任... 详细信息

农地确权的经济影响效应受到了学界的广泛关注,但鲜有研究关注农地确权政策的政治效应。基于3期农地确权追踪调查数据,利用广义DID模型评估农地确权对农户政治信任水平的影响。结果表明:农地确权使农户的中央级政治信任、村级政治信任分别提升0.142个单位和0.215个单位。上述结果在考虑平行趋势、样本随机性、控制潜在遗漏变量、替换被解释变量、更换计量模型后依然稳健。机制分析表明,农地确权通过降低地权权益的保护成本、提升盘活农地产权收益两条途径对农户政治信任产生影响。进一步分析显示:农地确权执行规范程度越高,不影响农户的中央级政治信任,但会显著提升农户的村级政治信任水平。由此认为,农地确权除产生经济影响外,也是政府投资农户政治信任的有效途径。

关键词：公共政策制度绩效农地确权产权保障政治信任

Essential factors of Sui Zheng Shi Liang strategy in Type 2 diabetes treatment assessed by questionnaire

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Journal of Traditional Chinese Medicine 2013年第1期33卷 27-33页

作者： Fengmei Lian xinyan chen Linhua Zhao Lipeng Xu Xiaolin Tong Endocrinology Department Guang'anmen Hospital China Academy of Chinese Medical Sciences

OBJECTIVE: Sui Zheng Shi Liang strategy (regulating prescription dosage with different syndromes) is an important part of syndrome differentiation and treatment in Traditional Chinese Medicine (TCM). Questionnaires were given to doctors and patients to study the essential factors (indicators and timing) of Sui Zheng Shi Liang strategy in the treatment process of type 2 diabetes (T2DM). METHODS: Two questionnaires were designed for diabetes patients and their doctors. The questionnaires included the most important indicators for determining the patient's condition, the ability of TCM in treating T2DM, the length of time it takes for TCM to be effective, and when to adjust the prescription dosage.The frequency of answers was calculated, summarized, and analyzed after the survey. RESULTS: Twenty questionnaires from doctors and 90 questionnaires from patients were included in the analysis. Doctors and patients recognized thatTCM could decrease blood glucose, improve syndromes, and delay complications. Doctors were mainly concerned about glycosylated hemoglobin, while the patients were concerned about fasting plasma glucose for determining whether treatment was effective. Doctors also paid attention to changes in blood sugar and syndromes 2 weeks after medication was given as the indication to adjust the prescription dosage, while patients were concerned about these factors in 4 weeks.The prescription should be regulated when there are side effects or the medication is ineffective. CONCLUSION: The essential factor in the treatment process of T2DM in Sui Zheng Shi Liang strategy is that if fasting blood glucose level did not decrease after 4 weeks of treatment, the Chinese medicine prescription should be adjusted.

关键词： 2型糖尿病药物治疗问卷调查中国传统医学中药处方评估糖化血红蛋白空腹血糖

Three-month effects of corneal cross-linking on corneal fibroblasts

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BIOCELL 2021年第4期45卷 1023-1032页

作者： xinyan chen HAIXIA ZHANG LIN LI School of Biomedical Engineering Capital Medical UniversityBeijing100069China Beijing Key Laboratory of Fundamental Research on Biomechanics in Clinical Application Capital Medical UniversityBeijing100069China

Corneal collagen crosslinking(CXL)has revolutionized the treatment of keratoconus in the past decade.In order to evaluate the 3-month effects of CXL on corneal fibroblasts,a longitudinal study at the tissue and cellular level was carried out with a total of 16 rabbits that underwent CXL,deepithelialization(DEP),or non-treatment(control)and kept for 1 to 3 months.The duration of corneal stromal remodeling after CXL was determined by examining the differentiation,apoptosis,and number changes of keratocytes in tissue sections from animals 1,2,or 3 months post-treatment.Upon the finish of tissue remodeling,separate rabbits were used to extract keratocytes and set up cell culture for vimentin immunofluorescence staining.The same cell culture was used for(1)migration measurement through the wound-healing assay;(2)elastic modulus measurement by atomic force microscope(AFM);(3)the proliferation,apoptosis,cytoskeleton andα-SMA expression tests through EdU(5-ethynyl-2’-deoxyuridine)assay,TUNEL(TdT-mediated dUTP Nick-End Labeling)assay,phalloidin andα-SMA(alpha-smooth muscle actin)immunofluorescence analysis,respectively.Results showed that the migratory activity,elastic modulus,andα-SMA expression of the corneal fibroblasts increased after CXL treatment,while apoptosis,proliferation,and morphology of F-actin cytoskeleton of the fibroblasts had no significant change after 3 months.In contrast,measured cellular parameters(migratory,elastic moduli,α-SMA expression,apoptosis,proliferation,and morphology of F-actin cytoskeleton of fibroblasts)did not change significantly after DEP.In conclusion,the dynamic changes of keratocytes were nearly stable 3 months after CXL treatment.CXL has an impact on corneal fibroblasts,including migration,elastic modulus andα-SMA expression,while epithelialization may not alter the biological behavior of cells significantly.

关键词： CXL Elastic modulus Stromal remodeling Mechanobiological behavior

Immobilized laccase on magnetic nanoparticles for enhanced lignin model compounds degradation

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Chinese Journal of Chemical Engineering 2020年第8期28卷 2152-2159页

作者： xinyan chen Bin He Mi Feng Dingwei Zhao Jian Sun Key Laboratory of Molecular Medicine and Biotherapy School of Life ScienceBeijing Institute of TechnologyBeijing 100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China

As a natural aromatic polymer,lignin has great potential but limited industrial application due to its complex chemical structure.Among strategies for lignin conversion,biodegradation has attracted promising interest recently in term of efficiency,selectivity and mild condition.In order to overcome the issues of poor stability and non-reusability of enzyme in the biodegradation of lignin,this work explored a protocol of immobilized laccase on magnetic nanoparticles(MNPs)with rough surfaces for enhanced lignin model compounds degradation.Scanning electron microscope with energy dispersive spectrometer(SEM-EDS),flourier transformation infrared spectroscopy(FTIR)and thermal gravimetric analysis(TGA)were utilized to characterize the immobilization of laccase.The results showed a maximum activity recovery of 64.7%towards laccase when it was incubated with MNPs and glutaraldehyde(GA)with concentrations of 6 mg·ml^-1and 7.5 mg·ml^-1for 5 h,respectively.The immobilized laccase showed improved thermal stability and pH tolerance compared with free laccase,and remained more than 80%of its initial activity after 20 days of storage at 4℃.In addition,about 40%residual activity of the laccase remained after 8 times cycles.Gas chromatography–mass spectrometry(GC–MS)was utilized to characterize the products of lignin model compound degradation and activation,and the efficiency of immobilized laccase was calculated to be 1–5 times that of free laccase.It was proposed that the synergistic effect between MNPs and laccase displays an important role in the enhancement of stability and activity in lignin model compound biodegradation.

关键词： Laccase Immobilization Magnetic nanoparticles Lignin model compounds Degradation