通讯机构：
[Qiu, S ] Z;[Li, JR; Sun, Y ] C;[Xiong, XX ] W;Zhejiang Univ, Huzhou Cent Hosp, Affiliated Huzhou Hosp, Dept Neurosurg,Sch Med, Huzhou 313000, Peoples R China.;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticides, Wuhan 430079, Peoples R China.
关键词：
Metallacycles;metallacages;Near-infrared biochannel;In vivo imaging;Theranostic
摘要：
In the past decade, the metallacycles/metallacages have attracted unremitting interest in biomedical fields, yet visual tracking of their in vivo delivery, targeting ability, biodistribution and therapeutic evaluation are still hampered by their short emission wavelengths. More recently, the near-infrared biochannel (NIR, 0.7-1.7 & mu;m) especially the NIR-II region (1.0-1.7 & mu;m) provides deeper tissue penetration and higher contrast than traditional UV-Vis region for in vivo imaging. In this context, we provide a comprehensive and systematic insight into the development of NIR metallacycles/metallacages for biomedical applications. Finally, we also discuss the challenges and prospects of NIR metallacycles/metallacages for future biomedical research and clinical translation.
作者机构：
[Feng, Guoqiang; Li, Qianhua; Gong, Shengyi; Jiang, Siyu; Zhu, Wenlong] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Guoqiang Feng] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan 430079, China
通讯机构：
[Hongwei Sun; Zhihui Ai] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental Chemistry, Central China Normal University, Wuhan 430079, PR China
关键词：
Heterogeneous fenton reaction;Oxalic acid;Proton transfer;Thiamphenicol;Zero-valent iron
摘要：
Heterogeneous Fenton reactions of zero-valent iron (ZVI) requires the sufficient release of Fe(II) to catalyze the H(2)O(2) decomposition. However, the rate-limiting step of proton transfer through the passivation layer of ZVI restricted the Fe(II) release via Fe(0) core corrosion. Herein we modified the shell of ZVI with highly proton-conductive FeC(2)O(4)·2H(2)O by ball-milling (OA-ZVI(bm)), and demonstrated its high heterogeneous Fenton performance of thiamphenicol (TAP) removal, with 500 times enhancement of the rate constant. More importantly, the OA-ZVI(bm)/H(2)O(2) showed little attenuation of the Fenton activity during 13 successive cycles, and was applicable across a wide pH range of 3.5-9.5. Interestingly, the OA-ZVI(bm)/H(2)O(2) reaction showed pH self-adapting ability, which initially reduced and then sustained the solution pH in the range of 3.5-5.2. The abundant intrinsic surface Fe(II) of OA-ZVI(bm) (45.54% vs. 27.52% in ZVI(bm), according to Fe 2p XPS profiles) was oxidized by H(2)O(2) and hydrolyzed to generate protons, and the FeC(2)O(4)·2H(2)O shell favored the fast transfer of protons to inner Fe(0), therefore, the consumption-regeneration cycle of protons were accelerated to drove the production of Fe(II) for Fenton reactions, demonstrated by the more prominent H(2) evolution and nearly 100% H(2)O(2) decomposition by OA-ZVI(bm). Furthermore, the FeC(2)O(4)·2H(2)O shell was stable and slightly decreased from 1.9% to 1.7% after the Fenton reaction. This study clarified the significance of proton transfer on the reactivity of ZVI, and provided an efficient strategy to achieve the highly efficient and robust heterogeneous Fenton reaction of ZVI for pollution control.
作者机构：
Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China;School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore, Singapore;[Tierui Zhang; Tierui Zhang Tierui Zhang Tierui Zhang] Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, China;[Jinyu Yan; Yuan Li; Shuxin Ouyang; Jinyu Yan Jinyu Yan Jinyu Yan; Yuan Li Yuan Li Yuan Li; Shuxin Ouyang Shuxin Ouyang Shuxin Ouyang] Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China
通讯机构：
[Shuxin Ouyang; Shuxin Ouyang Shuxin Ouyang Shuxin Ouyang] E;[Tierui Zhang; Tierui Zhang Tierui Zhang Tierui Zhang] K;Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, China<&wdkj&>Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, China
摘要：
We classify the representative photocatalytic materials for photosynthesis of hydrogen peroxide (H2O2) in recent years and discuss the related modification methods in detail, providing inspiration and insights for the future design of photocatalysts for H2O2 production. Abstract Hydrogen peroxide (H2O2), an environmental‐friendly oxidant and renewable liquid fuel, has received wide attention in various research and industrial fields. Current industrial production of H2O2 relies on the anthraquinone method, which is hardly viewed as a sustainable and green process. Photocatalysis, harnessing solar energy as the driving force for redox reactions, provides a green and promising approach for H2O2 production. However, due to the poor ability of light absorption, fast recombination of carriers, and poor intrinsic activity of active sites of pristine photocatalysts, photocatalytic H2O2 production cannot provide great yield. Thus, great efforts have been dedicated to design efficient photocatalysts for photosynthesis of H2O2 in the past decades. In this review, we summarize significant progress in the development of advanced photocatalytic materials for light‐driven H2O2 production. Starting with a brief introduction on basic principles and advantages of photosynthesis of H2O2, the representative materials are classified and discussed in detail; finally, a brief outlook on addressing future challenges and opportunities of photocatalytic H2O2 production is proposed. This review aims to confirm current challenges and research developments in the photosynthesis of H2O2 and provide inspiration for the development of high‐efficiency photocatalysts for photocatalytic H2O2 production in the future.
作者机构：
[Bao, Guang-Ming; Wang, Yongze; Luo, Xin; Li, Shentian] Hubei Univ Technol, Hubei Prov Cooperat Innovat Ctr Ind Fermentat, Natl Ctr Cellular Regulat & Mol 111, Hubei Res Ctr Food Fermentat Engn,Key Lab Fermenta, Wuhan 430068, Hubei, Peoples R China.;[Xu, Weiqing; Luo, Zhen; Fang, Qie; Zhu, Chengzhou; Gu, Wenling; Wang, Hengjia] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Zhu, CZ] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Zhu, CZ ] ;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
An amphiphilic AIE photosensitizer has been successfully developed, which allows for easily inserting into the bacterial membranes. Binding experiments with phospholipid preliminary demonstrates its membrane specificity. As expected, it is proved to possess a broad-spectrum bacterial staining performance and photodynamic antibacterial activity toward S. aureus and E. coli.
通讯机构：
[Shi-Yu Liu; Xianwang Wang] D;Department of Biochemistry and Molecular Biology, Center for Molecular Medicine, Health Science Center, Yangtze University, Jingzhou, Hubei, 434023, PR China<&wdkj&>Department of Laboratory Medicine, Health Science Center, Yangtze University, Jingzhou, Hubei, 434023, PR China<&wdkj&>Department of Biochemistry and Molecular Biology, Center for Molecular Medicine, Health Science Center, Yangtze University, Jingzhou, Hubei, 434023, PR China
关键词：
Cancer screening;Fluorescent probe;Leukotriene A4 hydrolase;Living imaging
摘要：
Early diagnosis of cancer is an efficient strategy to prevent tumor progression and improve the survival rate of patients. However, to discovery of reliable tumor-specific biomarkers remains a great challenge. Leukotriene A4 hydrolase (LTA(4)H) is a bifunctional zinc metalloenzyme with epoxide hydrolase activity and aminopeptidase activity, which plays important roles in allergic and inflammatory reactions and showed strong relevance with carcinoma progression. We thus sought to investigate the possibility of application LTA(4)H activity detection in cancer diagnosis. To achieve this, we herein develop an enzyme activated fluorescent probe for LTA(4)H activity sensing by incorporating the specific recognition unit of LTA(4)H with a red-emitting fluorophore. The acquired probe (named as ADMAB) showed high sensitivity and specificity toward LTA(4)H in vitro. By further application of ADMAB in living cells, significantly elevated LTA(4)H activity in cancer cell lines was observed when compared with normal cell lines and in vivo tracing A549 tumor in nude mice was also realized by ADMAB. Meanwhile, the wound-healing assay further revealed the importance of LTA(4)H in tumor metastasis. Moreover, the LTA(4)H activity in human serum sample was successfully detected by ADMAB and significantly elevated LTA(4)H activity in patients diagnosed with cancer was firstly found, which demonstrated ADMAB to be a useful tool for cancer diagnosis and LTA(4)H related biological study.
摘要：
AimThe urokinase plasminogen activator receptor (uPAR) is a promising biomarker for cancer diagnosis and therapy. We herein fabricated a new type of uPAR-targeted imaging probe (AlF)-F-18-NOTA-VC and preliminarily evaluated its potential application in PET imaging of the glioma model in vivo. MethodsPeptide VC was synthesized and identified by MALDI-TOF-MS. The IC50 between VC/precursor NOTA-VC and uPAR was then determined before the synthesis and purification of (AlF)-F-18-NOTA-VC, followed by further studies of in-vitro properties of (AlF)-F-18-NOTA-VC. Meanwhile, the AE105-based probe followed a similar procedure in-vitro test. Finally, the PET imaging properties, including uPAR-targeting ability and the metabolism of (AlF)-F-18-NOTA-VC, were investigated. ResultsThe VC and NOTA-VC were obtained successfully and demonstrated a good affinity with uPAR. Followed by (AlF)-F-18 labeling successfully, excellent properties, including the serum stability, water solubility, and specificity of (AlF)-F-18-NOTA-VC, were obtained in-vitro test compared with AE105 based probe. An excellent tumor uptake and renal excretion data of (AlF)-F-18-NOTA-VC were acquired from in-vivo U87MG tumor model PET imaging, consistent with the subsequent biodistribution study. ConclusionIn addition to the excellent specificity and high tumor/normal tissue contrast for uPAR-targeted PET imaging of U87MG tumor, (AlF)-F-18-NOTA-VC possessed promising clearance ability by renal system route. These excellent properties facilitated (AlF)-F-18-NOTA-VC to be a promising imaging agent for uPAR high-expressing tumors and, thus, provided a paradigm for developing peptide-based probes for uPAR-associated disease diagnosis.
摘要：
Inositol hexakisphosphate (IP6), a naturally occurring metabolite of inositol with specific functions in different organelles or tissues, participates in numerous physiological processes and plays a key role in mammalian metabolic regulation. However, current IP6 detection methods, i.e., high-performance liquid chromatography and gel electrophoresis, require sample destruction and lack spatiotemporal resolution. Here, we construct and characterize a genetically encoded fluorescence biosensor named HIPSer that enables ratiometric quantitative IP6 detection in HEK293T cells and subcellular compartments. We demonstrate that HIPSer has a high sensitivity and relative selectivity for IP6 in vitro. We also provide proof-of-concept evidence that HIPSer can monitor IP6 levels in real time in HEK293T cells and can be targeted for IP6 detection in the nucleus of HEK293T cells. Moreover, HIPSer could also detect changes in IP6 content induced by chemical inhibition of IP6-metabolizing enzymes in HEK293T cells. Thus, HIPSer achieves spatiotemporally precise detection of fluctuations in endogenous IP6 in live cells and provides a versatile tool for mechanistic investigations of inositol phosphate functions in metabolism and signaling.
通讯作者：
Xuan Jiang<&wdkj&>Prof. Liang-Qiu Lu<&wdkj&>Prof. Wen-Jing Xiao<&wdkj&>Xuan Jiang Xuan Jiang Xuan Jiang<&wdkj&>Prof. Liang-Qiu Lu Prof. Liang-Qiu Lu Prof. Liang-Qiu Lu<&wdkj&>Prof. Wen-Jing Xiao Prof. Wen-Jing Xiao Prof. Wen-Jing Xiao
作者机构：
[Yue Jia; Prof. Zhihan Zhang; Guo-Ming Yu; Xuan Jiang; Yue Jia Yue Jia Yue Jia; Prof. Zhihan Zhang Prof. Zhihan Zhang Prof. Zhihan Zhang; Guo-Ming Yu Guo-Ming Yu Guo-Ming Yu; Xuan Jiang Xuan Jiang Xuan Jiang] Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei, 430079 China;Wuhan Institute of Photochemistry and Technology, 7 North Bingang Rd., Wuhan, Hubei, 430082 China;State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, 345 Lingling Road, Shanghai, 200032 China;State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Lanzhou, 730000 China;School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, Henan, 453007 China
通讯机构：
[Xuan Jiang; Prof. Liang-Qiu Lu; Prof. Wen-Jing Xiao; Xuan Jiang Xuan Jiang Xuan Jiang; Prof. Liang-Qiu Lu Prof. Liang-Qiu Lu Prof. Liang-Qiu Lu; Prof. Wen-Jing Xiao Prof. Wen-Jing Xiao Prof. Wen-Jing Xiao] E;Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei, 430079 China<&wdkj&>Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei, 430079 China<&wdkj&>Wuhan Institute of Photochemistry and Technology, 7 North Bingang Rd., Wuhan, Hubei, 430082 China<&wdkj&>State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, 345 Lingling Road, Shanghai, 200032 China<&wdkj&>Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei, 430079 China<&wdkj&>State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Lanzhou, 730000 China<&wdkj&>School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, Henan, 453007 China
摘要：
The exploration of value-added conversions of naturally abundant amino acids has received considerable attention from the synthetic community. Compared with the well-established asymmetric decarboxylative transformation, the asymmetric deaminative transformation of amino acids still remains a formidable challenge, mainly due to the lack of effective strategies for the C−N bond activation and the potential incompatibility with chiral catalysts. Here, we disclose a photoinduced Cu-catalyzed asymmetric deaminative coupling reaction of amino acids with arylboronic acids. This new protocol provides a series of significant chiral phenylacetamides in generally good yields and excellent stereoselectivity under mild and green conditions (42–85 % yields, up to 97 % ee). Experimental investigations and theoretical calculations were performed to reveal the crucial role of additional phenols in improving catalytic efficiency and enantiocontrol.
作者机构：
[Zhang, Qing-Pu; Sun, Yu-Ling; Ma, Hui; Wang, Zhen; Zhang, Chun; Yang, Bin-Bin] Huazhong Univ Sci & Technol, Coll Life Sci & Technol, Natl Engn Res Ctr Nanomed, Wuhan 430074, Peoples R China.;[Wang, Zhen] Wuhan Text Univ, Technol Inst, Natl Engn Lab Adv Yarn & Fabr Format & Clean Prod, Wuhan 430200, Hubei, Peoples R China.;[Meng, Xianggao] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.;[Zhang, Yaohua] Hubei Tobacco Grp Co Ltd, Technol R&D Ctr, Wuhan 430070, Peoples R China.
通讯机构：
[Zhang, Yaohua] T;[Meng, Xianggao; Sun, Yu-Ling] C;College of Life Science and Technology, National Engineering Research Center for Nanomedicine, Huazhong University of Science and Technology, Wuhan, 430074, China.;College of Chemistry, Central China Normal University, Wuhan, 430079, China.;Technology R&D Center, Hubei Tobacco (Group) Co., Ltd, Wuhan, 430070, China.
摘要：
A pair of chiral, emissive and porous tubular multi-functional organic molecular cages were synthesized easily by imine chemistry of 4,4′,4′′,4′′′-(ethene-1,1,2,2-tetrayl)-tetrabenzaldehyde (ETTBA) with (R,R)- or (S,S)-diaminocyclohexane (CHDA). It was found that the chirality of CHDA was transferred and amplified to tetraphenylethylene (TPE) in the process of formation of cages, which further endowed the cages with circularly polarized luminescence (CPL) characteristics. As a result of the synergy of the chirality and porous structure in the solid state, both cages exhibited a good chiral adsorption enantioselectivity to a series of aromatic racemates.
摘要：
Oxygen vacancies (O(V)), as the sites of molecular oxygen adsorption and activation, play an important role in the catalytic combustion process of volatile organic compounds (VOCs). Revealing the relationship between O(V) concentration and molecular oxygen activation behavior is of significance to construct the efficient catalysts. Herein, α-MnO(2) with different O(V) concentrations was prepared to investigate the molecular oxygen activation for C(3)H(8) combustion. It is disclosed that the enhanced O(V) concentration in α-MnO(2) induced the reconfiguration of surface metal atoms, resulting in the transformation of oxygen activation configuration from end-on mode to side-on mode. Oxygen molecules in side-on mode possessed more localized electron density and weaker coordination bond strength with surrounding Mn atoms, which were more favorable to adsorb C(3)H(8) molecules and activate C-H bond for the improved combustion performance. This work provides a new understanding to reveal that the increased O(V) concentration contributes to more efficient VOCs combustion.
作者机构：
[Xu, Guang; Chen, Jian; Yu, Hong; Liu, Jinpeng; Yin, Tingrui; Meng, Sixuan; Zhang, Ying; Yu, Guang-Ao] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Lin, Xiuhua; Dang, Li; Dang, L] Shantou Univ, Dept Chem, Shantou 515063, Guangdong, Peoples R China.;[Lin, Xiuhua; Dang, Li; Dang, L] Shantou Univ, Key Lab Preparat & Applicat Ordered Struct Mat Gua, Shantou 515063, Guangdong, Peoples R China.;[Lin, Xiuhua; Dang, Li; Dang, L] Chem & Chem Engn Guangdong Lab, Shantou 515063, Guangdong, Peoples R China.;[Yuan, Jia; Yuan, J] Wuhan Text Univ, State Key Lab New Text Mat & Adv Proc Technol, Wuhan 430200, Peoples R China.
通讯机构：
[Yuan, J ] W;[Yu, GA ] C;[Dang, L ] S;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Shantou Univ, Dept Chem, Shantou 515063, Guangdong, Peoples R China.
摘要：
We developed the remote selective C-H bromination for the synthesis of C4 & PRIME;-brominated biarylphosphine oxides using FeBr3 as a brominating reagent. C3 & PRIME;-Brominated products were obtained in reactions with substrates bearing a 2,4,6-triisopropyl substituent on the bottom ring. Moreover, direct access to C5-chlorinated peri-substituted(1-naphthalenyl)phosphines is developed using FeCl3 as a chlorinating reagent. These halogenated compounds can be utilized for cross-coupling reactions to construct functionalized phosphine oxides.
通讯机构：
[Chen, JR ] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol, Minist Educ, Wuhan, Hubei, Peoples R China.;Wuhan Inst Photochem & Technol, Wuhan, Hubei, Peoples R China.
摘要：
Lactams and pyridines are privileged scaffolds, but strategies for combining these groups into one molecule are lacking. Now, N-N pyridinium ylides have been shown to form triplet state diradicals under photoinduced energy transfer, and subsequent [3+2] cycloaddition with the tethered alkene enables the synthesis of diverse ortho-pyridyl lactams.
