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Hierarchically porous metal–organic frameworks:synthetic strategies and applications

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National Science Review 2020年第11期7卷 1743-1758页

作者： Liang Feng Kun-Yu Wang Xiu-Liang Lv Tian-Hao Yan hong-cai zhou Department of Chemistry Texas A&M UniversityCollege Station Department of Materials Science and Engineering Texas A&M UniversityCollege Station

Despite numerous advantages, applications of conventional microporous metal–organic frameworks (MOFs) are hampered by their limited pore sizes, such as in heterogeneous catalysis and guest delivery,which usually involve large molecules. Construction of hierarchically porous MOFs (HP-MOFs) is vital to achieve the controllable augmentation of MOF pore size to mesopores or even macropores, which can enhance the diffusion kinetics of guests and improve the storage capacity. This review article focuses on recent advances in the methodology of HP-MOF synthesis, covering preparation of HP-MOFs with intrinsic hierarchical pores, and modulated, templated and template-free synthetic strategies for *** key factors which affect the formation of HP-MOF architectures are summarized and discussed,followed by a brief review of their applications in heterogeneous catalysis and guest encapsulation. Overall,this review presents a roadmap that will guide the future design and development of HP-MOF materials with molecular precision and mesoscopic complexity.

关键词： metal–organic frameworks hierarchical design synthesis application

Nitrogen-rich porphyrinic metal-organic frameworks synthesized by postsynthetic metathesis: from inert material to active catalyst

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Science China Chemistry 2016年第8期59卷 975-979页

作者： Dahuan Liu Xuan Wang Ying-Pin Chen Shuai Yuan Chongli Zhong hong-cai zhou Department of Chemistry Texas A&M University College Station Texas 77843-3255 USA State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 China Department of Material Science and Engineering Texas A&M University College Station Texas 77842 USA

With the aid of a postsynthetic metathesis method, an inert nitrogen-rich porphyrinic metal-organic framework can exhibit a high catalytic activity in one-pot deacetalization-Knoevenagel condensation reaction.

关键词： metal-organic frameworks porous coordination network post-synthetic metathesis catalysis tetrazolate

Lactonization of dyes promoted by a coordination cage facilitates cavity-induced chromism as ion mobile detector

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Science China Chemistry 2024年第5期67卷 1554-1560页

作者： Liangliang Zhang Yu Liang Zhifeng Xiao Yuxuan Meng Jinyi Huang Xi Lin Ji Li hong-cai zhou Yu Fang Strait Institute of Flexible Electronics(SIFE Future Technologies)Fujian Normal University and Strait Laboratory of Flexible Electronics(SLoFE)Fuzhou 350017China State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Department of Chemistry Texas A&M UniversityCollege StationTexas 77842-3012USA State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Frontiers Science Center for Flexible Electronics(FSCFE) MIIT Key Laboratory of Flexible Electronics(KLoFE)Northwestern Polytechnical UniversityXi’an 710072China

Dye molecules often change colors(so-called “chromism”) according to the environment variation. However, they are rarely induced by a catalytic amount of cavity. Through encapsulation in the cavity of a porous coordination cage(PCC-2), Rhodamine B(1) is transformed from red quinonoid form(1q) into colorless lactone form(1l) in aprotic polar solutions. The μ4-OH groups in the cavity of PCC-2 are shown to stabilize the uncommon zwitterion intermediate(1z), followed by converting to 1l, thus accelerating the equilibrium. The chromism is catalyzed by 0.25 mol% of PCC-2, and the reaction rate is improved by 80,400times. 1@PCC-2 can be further fabricated to a sol-gel that exhibits ion recognition properties. The resulting encapsulation and stabilization of an unconventional intermediate by a catalytic amount of the coordination cage provides fundamental insights into molecular isomerization and has potential use in chemical sensing.

关键词： porous coordination cage Zwitterion intermediate cavity Rhodamine B chromism

AP-2α expression and cell apoptosis of the lung tissue of rats with COPD and ECV304 cells stimulated by cigarette smoke extract

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Chinese Science Bulletin 2011年第15期56卷 1562-1568页

作者： LI JunLi CHEN Yan CHEN Ping cai Shan PENG hong zhou Rui XIANG XuDong LONG hong LIU ShaoKun Department of Respiratory Medicine Xiangya Second Hospital of Central South University Changsha Hunan 410011 China

An increasing body of evidence suggests that apoptosis of structural cells in the lung might be an important upstream event in the pathogenesis of chronic obstructive pulmonary disease (COPD).AP-2α is one of the important transcription factors involved in the modulation of apoptosis in carcinogenesis and idiopathic-dilated *** relationship between AP-2α and apoptosis in COPD remains to be *** aim of the present study was to investigate the expression of AP-2α in the lung tissues of rats with COPD induced by smoking and its possible protective effect on cigarette smoke extract (CSE) induced endothelial cell ***-Dawley rats (n=24) were randomly assigned to normal and COPD *** COPD group was exposed to smoke from 20 commercial unfiltered cigarettes for 80 d before morphological assessment of the lung tissue was *** expression of AP-2α in lung tissues was measured by Western *** demonstrate the relationship between apoptosis and AP-2α,in vitro cell experiments were carried *** were treated with different concentrations of CSE before proliferation was measured by *** was then determined by Hoechst staining and the expression of cleaved caspase-3 and AP-2α by Western blotting over time following treatment with 5% *** were then infected with an AP-2α adenovirus vector and the expression of cleaved caspase-3 and AP-2α was compared to the control groups by Western *** COPD group showed larger air spaces and significant decrease of FEV 0.3/FVC compared with the rats in the control group (P<0.05).The expression of AP-2α was significantly higher in the lung tissue of rats with COPD compared with those of controls (P<0.05).In the ECV304 cells,CSE induced apoptosis (P<0.01) and caspase-3 activation in a time-dependent manner and reduced the cell proliferation rate in a dose-dependent manner (P<0.005).Moreover,5% CSE treatment increased endogenous AP-2α protein ***-2α overexpr

关键词：慢性阻塞性肺病细胞凋亡香烟烟雾提取物 AP 大鼠 caspase 癌组织

Combined TIM-3 and PD-1 blockade restrains hepatocellular carcinoma development by facilitating CD4+ and CD8+T cellmediated antitumor immune responses

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World Journal of Gastrointestinal Oncology 2023年第12期15卷 2138-2149页

作者： Xu-Sheng Zhang hong-cai zhou Peng Wei Long Chen Wei-Hu Ma Lin Ding Shi-cai Liang Ben-Dong Chen School of Clinical Medicine Ningxia Medical UniversityYinchuan 750004Ningxia Hui Autonomous RegionChina Department of Hepatobiliary Surgery The General Hospital of Ningxia Medical UniversityYinchuan 750004Ningxia Hui Autonomous RegionChina Hepatobiliary Pancreatic Surgical Ningxia Hepatobiliary Pancreatic Surgical Diseases Clinical Research CenterYinchuan 750004Ningxia Hui Autonomous RegionChina

BACKGROUND Immune checkpoint inhibitors(ICIs)targeting programmed cell death protein 1(PD-1)and T cell immunoglobulin and mucin domain-containing protein 3(TIM-3)are beneficial to the resumption of anti-tumor immunity response and hold extreme potential as efficient therapies for certain ***,ICIs with a single target exhibit poor overall response rate in hepatocellular carcinoma(HCC)patients due to the complex pathological mechanisms of *** To investigate the effects of combined TIM-3 and PD-1 blockade on tumor development in an HCC mouse model,aiming to identify more effective immunotherapies and provide more treatment options for HCC *** The levels of PD-1 and TIM-3 on CD4+and CD8+T cells from tumor tissues,ascites,and matched adjacent tissues from HCC patients were determined with flow *** HCC xenograft mouse model was established and treated with anti-TIM-3 monoclonal antibody(mAb)and/or anti-PD-1 *** growth in each group was *** and eosin staining and immunohistochemical staining were used to evaluate T cell infiltration in *** percentage of CD4+and CD8+T cells in tissue samples from mice was tested with flow *** percentages of PD-1+CD8+,TIM-3+CD8+,and PD-1+TIM-3+CD8+T cells was accessed by flow *** levels of the cytokines including tumor necrosis factor alpha(TNF-α),interferon-γ(IFN-γ),interleukin(IL)-6,and IL-10 in tumor tissues were gauged with enzyme-linked immunosorbent assay *** We confirmed that PD-1 and TIM-3 expression was substantially upregulated in CD4+and CD8+T cells isolated from tumor tissues and ascites of HCC ***-3 mAb and PD-1 mAb treatment both reduced tumor volume and weight,while combined blockade had more substantial anti-tumor effects than individual *** we showed that combined therapy increased T cell infiltration into tumor tissues,and downregulated PD-1 and TIM-3 expression on CD8+T cells in tumor ***,c

关键词： Hepatocellular carcinoma T cell immunoglobulin and mucin domain-containing protein 3 Programmed cell death protein 1 CD4+T cells CD8+T cells

Multielectron transportation of polyoxometalate-grafted metalloporphyrin coordination frameworks for selective CO2-to-CH4 photoconversion

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National Science Review 2020年第1期7卷 53-63页

作者： Qing Huang Jiang Liu Liang Feng Qi Wang Wei Guan Long-Zhang Dong Lei Zhang Li-Kai Yan Ya-Qian Lan hong-cai zhou Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials Science Nanjing Normal University Department of Chemistry Texas A&M University College Station Department of Chemistry Northeast Normal University

Photocatalytic CO2reduction into energy carriers is of utmost importance due to the rising concentrations of CO2and the depleting energy resource. However, the highly selective generation of desirable hydrocarbon fuel, such as methane（CH4）, from CO2remains extremely challenging. Herein, we present two stable polyoxometalate-grafted metalloporphyrin coordination frameworks（POMCFs）, which are constructed with reductive Zn-ε-Keggin clusters and photosensitive tetrakis（4-carboxylphenyl）porphyrin（H2TCPP） linkers, exhibiting high selectivity（>96%） for CH4formation in a photocatalytic CO2-reduction system. To our knowledge, the high CH4selectivity of POMCFs has surpassed all of the reported coordination-framework-based heterogeneous photocatalysts for ***, the introduction of a Zn-ε-keggin cluster with strong reducing ability is the important origin for POMCFs to obtain high photocatalytic selectivity for CH4formation, considering that eight MoVatoms can theoretically donate eight electrons to fulfill the multielectron reduction process of CO2-to-CH4transformation.

关键词： reductive polyoxometalate coordination frameworks CO2 photoreduction high selectivity methane

Outcomes of transconjunctival sutureless 27-gauge vitrectomy for vitreoretinal diseases

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International Journal of Ophthalmology(English edition) 2018年第3期11卷 408-415页

作者： Jie Li San-Mei Liu Wen-Tao Dong Fang Li cai-hong zhou Xiao-Dan Xu Jie Zhong Department of Ophthalmology Sichuan Academy of Medical Science & Sichuan Provincial People's Hospital School of Medicine University of Electronic Science and Technology of China

AIM： To evaluate the safety and efficacy profile of 27-gauge （27G） pars plana vRrectomy （PPV） for the treatment of various vitreoretinal diseases. METHODS： The clinical outcomes of 61 eyes （58 patients） with various vitreoretinal diseases following 27G PPV were retrospectively reviewed. RESULTS： Surgical indications included rhegmatogenous retinal detachment （n=24）, full-thickness macular hole （n=12）, diabetic retinopathy （n=11）, vitreous hemorrhage （n=6）, Eales disease （n=4）, pathological myopia-related vitreous floater （n=2）, and macular epiretinal membrane （n=2）. The mean follow-up was 166.4±61.3d （range 98-339d）. The mean IogMAR best-corrected visual acuity （BCVA） improved from 1.7±1.1 [0.02 decimal visual acuity （VA） equivalent] preoperatively to 1.2±1.0 （0.06 decimal VA equivalent） at the last postoperative visit （P〈0.001）. The mean operative time was ***. With the exception of complicated cataract in one eye, no intraoperative complications were encountered. No case required conversion to conventional 20-, 23- or 25G instrumentation in all surgical maneuvers except for silicone oil infusion, which required a 25G oil injection syringe. Postoperative complications included transient ocular hypertension, vitreous hemorrhage, persistent intraocular pressure elevation, subconjunctival oil leakage, and recurrent retinal detachment. No cases of hypotony, endophthalmitis, and sclerotomy-related tears were observed. CONCLUSION： The current results suggest that 27G PPV system is a safe and effective treatment for various vitreoretinal diseases. When learning to perform 27G PPV,surgeons may encounter a learning curve and should gradually expand surgical indications from easy to pathologically complicated cases.

关键词： 27-gauge par plana vitrectomy vitreoretinaldisease

Tuning the Structure of Fe-Tetracarboxylate Frameworks Through Linker-Symmetry Reduction

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CCS Chemistry 2021年第2期3卷 1701-1709页

作者： Jiandong Pang Christina T.Lollar Sai Che Jun-Sheng Qin Jialuo Li Peiyu cai Mingyan Wu Daqiang Yuan Maochun hong hong-cai zhou Department of Chemistry Texas A&M UniversityCollege StationTX 77843-3255 State Key Laboratory of Structure Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryInternational Center of Future ScienceJilin UniversityChangchun 130012 University of Chinese Academy of Sciences Beijing 100049

The design and synthesis of stable metal–organic frameworks(MOFs)have been a core obstacle in the widespread application of these functional crystalline porous materials,because of the stability limitations of MOFs under harsh operating ***,a highly stable microporous MOF based on the Fe_(3)O cluster(PCN-678)has been synthesized using a tetracarboxylate *** symmetry reduced tetratopic carboxylate ligand,a mesoporous MOF(PCN-668)could be obtained in which nanoscale cage-like building units and one-dimensional(1D)channels *** neighboring cages were mutual diastereomers in PCN-668 due to the further reduction of the Cs symmetry of the free ligand to C1 symmetry after ***,the acid stability of this mesoporous MOF was improved via postsynthetic metal exchange to chromium(PCN-668-Cr).The PCN-668-Cr exhibited very high stability in both acidic and basic aqueous solutions(pH=1–11).Additionally,the mesoporous MOF showed a high total gravimetric methane uptake(∼500 cm^(3) g^(−1) at 100 bar),while the microporous MOF showed a high volumetric methane storage capacity of 147 cm3 cm−3 at room temperature.

关键词： metal–organic framework mesoporous,highly stable diastereomeric cage methane uptake

Effects of hydrogen peroxide on mitochondrial gene expression of intestinal epithelial cells

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World Journal of Gastroenterology 2002年第6期8卷 1117-1122页

作者： Jian-Ming Li Qian cai hong zhou Guang-Xia Xiao,Institute of Burn Research,Southwest Hospital,Third Military Medical University,Chongqing 400038,China Institute of Burn Research Southwest Hospital Third Military Medical University Chongqing 400038 China.

AIM: To study the effects of hydrogen peroxide on mitochondrial gene expression of intestinal epithelial cells in in vitro model of hydrogen peroxide-stimulated SW-480 ***: RNA of hydrogen peroxide-induced SW-480 cells was isolated, and reverse-transcriptional polymerase chain reaction was performed to study gene expression of ATPase subunit 6, ATPase subunit 8, cytochrome c oxidase subunit Ⅰ (COⅠ), cytochrome coxidase subuit Ⅱ (COⅡ) and cytochrome c oxidase subunit Ⅲ (COⅢ). Mitochondria were isolated and activities of mitochondrial cytochrome c oxidase and ATPase were also measured ***: Hydrogen peroxide led to differential expression of mitochondrial genes with some genes up-regulated or down-regulated in a dose dependent manner. Differences were very obvious in expressions of mitochondrial genes of cells treated with hydrogen peroxide in a concentration of 400 μmol/L or 4 mmol/L. In general, differential expression of mitochondrial genes was characterized by up-regulation of mitochondrial genes in the concentration of 400 μmol/L and down-regulation in the concentration of 4 mmol/L. In consistence with changes in mitochondrial gene expressions, hydrogen peroxide resulted in decreased activities of cytochrome c oxidase and ***: The differential expression of mitochondrial genes encoding cytochrome c oxidase and ATPase is involved in apoptosis of intestinal epithelial cells by affecting activities of cytochorme c oxidase and ATPase.

关键词：过氧化氢小肠上皮细胞线粒体基因表达烧伤