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Chinese Journal of Chemical Engineering 2024年第4期68卷 231-240页

作者： Peng Jiang Hao Zhang Guanhan Zhao Lin Li Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu State Key Laboratory of Materials-oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream *** study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen *** this,process optimization and energy integration were implemented to provide optimized operation ***,a life cycle assessment was carried out to assess the carbon footprint of the coupled *** reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous *** optimizing systemic energy through heat integration,an energy efficiency of 86.30%was ***,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.

关键词： Biomass CaCO_(3)reductive calcination Chemical looping Hydrogen production Carbon footprint Thermodynamics process

Pairing nitroxyl radical and phenazine with electron-withdrawing/-donating substituents in “water-in-ionic liquid” for high-voltage aqueous redox flow batteries

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Green Energy & Environment 2024年第4期9卷 713-722页

作者： Zhifeng Huang Rolf Hempelmann Yiqiong Zhang Li Tao Ruiyong Chen Transfercenter Sustainable Electrochemistry Saarland University and KIST Europe66125SaarbruckenGermany State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical Engineering Hunan University Changsha410082HunanChina College of Materials science and Engineering Changsha University of science and Technology Changsha410114HunanChina Materials Innovation Factory Department of ChemistryUniversity of LiverpoolLiverpoolL697ZDUnited Kingdom

Aqueous redox-active organic materials-base electrolytes are sustainable alternatives to vanadium-based electrolyte for redoxﬂow batteries(RFBs)due to the advantages of high ionic conductivity,environmentally benign,safety and low ***,the underexplored redox properties of organic materials and the narrow thermodynamic electrolysis window of water(1.23 V)hinder their wide ***,seeking suitable organic redox couples and aqueous electrolytes with a high output voltage is highly suggested for advancing the aqueous organic *** this work,the functionalized phenazine and nitroxyl radical with electron-donating and electron-withdrawing group exhibit redox potential of-0.88 V and 0.78 V ***,respectively,in“water-in-ionic liquid”supporting *** spectra reveal that the activity of water is largely suppressed in“water-in-ionic liquid”due to the enhanced hydrogen bond interactions between ionic liquid and water,enabling an electrochemical stability window above 3 V.“Water-in-ionic liquid”supporting electrolytes help to shift redox potential of nitroxyl radical and enable the redox activity of functionalized *** assembled aqueous RFB allows a theoretical cell voltage of 1.66 V and shows a practical discharge voltage of 1.5 V in the“water-in-ionic liquid”***,capacity retention of 99.91%per cycle is achieved over 500 charge/discharge cycles.A power density of 112 mW cm^(-2) is obtained at a current density of 30 mA cm^(-2).This work highlights the importance of rationally combining supporting electrolytes and organic molecules to achieve high-voltage aqueous RFBs.

关键词： Aqueous redoxﬂow batteries Water-in-ionic liquid electrolytes High-voltage aqueous batteries Organic redox-active materials

Covalent triazine frameworks modified by ultrafine Pt nanoparticles for efficient photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 4908-4915页

作者： Xu Han Xueying Ge Wen-Wen He Wangwang Shen Tao Zhou Jian-Sen Wang Rong-Lin Zhong Abdullah MAl-Enizi Ayman Nafady Shengqian Ma School of Chemistry and Life science Advanced Institute of Materials ScienceChangchun University of TechnologyChangchun 130012China Laboratory of Theoretical and Computational Chemistry Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China Department of Chemistry University of North Texas1508 W.Mulberry St.DentonTX 76201USA Department of Chemistry College of ScienceKing Saud UniversityRiyadh 11451Saudi Arabia

Pt nanoparticles(PtNPs)as active species have always been considered as one of the best semiconductor materials for photocatalytic hydrogen *** this study,a Schottky heterojunction has been successfully constructed by evenly loading ultrafine PtNPs onto a triazine-based covalent organic frameworks(COFs).This strategy maintained the high activity of these ultra-small PtNPs while maximizing the utilization of the Pt active *** fabricated PtNPs@covalent triazine-based framework-1(CTF-1)composite accomplished a significantly high rate of hydrogen evolution(20.0 mmol·g^(−1)·h^(−1),apparent quantum efficiency(AQE)=7.6%,atλ=450 nm)with 0.40 wt.%Pt loading,giving rise to a 44-fold-increase in the efficiency of the photocatalytic hydrogen production compared to the pristine *** calculations revealed that the strong electron transfer(Q(Pt)=−0.726 qe,in the analysis of Bader charge,Q(Pt)is the charge quantity transferred from Pt cluster to CTF-1,and qe is the unit of charge transfer quantity)between PtNPs and CTF-1 triggers a strong interaction,which makes PtNPs being firmly attached to the structure of CTF-1,thereby enabling high stability and excellent hydrogen production ***,the hydrogen binding free energy(ΔGH*)of PtNPs@CTF-1 is much lower than that of the unmodified CTF-1,leading to a much lower intermediate state and hence a significant improvement in photocatalytic *** overall findings of this work provide a new platform to incorporate metallic NPs into COFs for the design and fabrication of highly efficient photocatalysts.

关键词： Pt nanoparticles covalent triazine-based framework-1(CTF-1) photocatalysts hydrogen evolution reaction

Eco-Friendly Encapsulation of Metal Clusters in Porous Organic Cages for Engineerable Microenvironment and Enhanced Catalysis

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CCS Chemistry 2024年第9期6卷 2186-2197页

作者： Siyu Ren Liangxiao Tan Jun-Hao Zhou Jian Sun Peng Zhang Xingzhong Cao Yun-Hong Zhang Jian-Ke Sun MOE Key Laboratory of Cluster science Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488 Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049

Developing artificial catalysts that mimic the functionality of enzymes and adapt to the surrounding microenvironment to achieve specific activity and selectivity is a fascinating research area yet remains a great *** this work,we present a meticulously designed strategy for the successful encapsulation of ultrasmall metal clusters(MCs)within an amine-type porous organic cage(POC)through electrostatic complexation,phase transfer,and alcohol reduction *** amine cage showcases an intriguing and customizable feature that allows for the regulation of the surrounding microenvironment of the confined MCs through a feasible postmodifi-cation *** functionalization of cage skeleton further facilitates precise adjustment to the surface electronic state of Pd cluster,thereby influencing the adsorption behavior of ***,this controlled regulation leads to modified activity and chemoselectivity in the catalytic hydrogenation of halogenated ***,the investigation of the correlation between the surrounding microenvironment,substrate adsorption,and catalytic performance in the POC-immobilized MCs system has not been previously *** anticipate that our research will provide valuable insights in this field.

关键词： metal cluster porous organic cage encapsulation microenvironment catalysis

Semi-implantable device based on multiplexed microfilament electrode cluster for continuous monitoring of physiological ions

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Bio-Design and Manufacturing 2024年第1期7卷 88-103页

作者： Shuang Huang Shantao Zheng Mengyi He Chuanjie Yao Xinshuo Huang Zhengjie Liu Qiangqiang Ouyang Jing Liu Feifei Wu Hang Gao Xi Xie Hui-jiuan Chen State Key Laboratory of Optoelectronic Materials and Technologies Guangdong Province Key Laboratory of Display Material and TechnologySchool of Electronics and Information TechnologySun Yat-Sen UniversityGuangzhou 510006China Guangdong Provincial Key Laboratory of Sensor Technology and Biomedical Instrument School of Biomedical EngineeringSun Yat-Sen UniversityShenzhen 518107China The First Affiliated Hospital of Sun Yat-Sen University Guangzhou 510080China Pazhou Lab Guangzhou 510335China Institute of Microelectronics of the Chinese Academy of sciences Beijing 100029China

Modern medicine is increasingly interested in advanced sensors to detect and analyze biochemical *** sensors based on potentiometric methods are a promising platform for monitoring physiological ions in biological *** semi-implantable devices are mainly based on single-parameter *** semi-implantable electrodes for multiparameter sensing have more restrictions on the electrode size due to biocompatibility considerations,but reducing the electrode surface area could potentially limit electrode *** study developed a semi-implantable device system comprising a multiplexed microfilament electrode cluster(MMEC)and a printed circuit board for real-time monitoring of intra-tissue K^(+),Ca^(2+),and Na^(+)*** electrode surface area was less important for the potentiometric sensing mechanism,suggesting the feasibility of using a tiny fiber-like electrode for potentiometric *** MMEC device exhibited a broad linear response(K^(+):2–32 mmol/L;Ca^(2+):0.5–4 mmol/L;Na^(+):10–160 mmol/L),high sensitivity(about 20–45 mV/decade),temporal stability(>2weeks),and good selectivity(>80%)for the above *** vitro detection and in vivo subcutaneous and brain experiment results showed that the MMEC system exhibits good multi-ion monitoring performance in several complex *** work provides a platform for the continuous real-time monitoring of ion fluctuations in different situations and has implications for developing smart sensors to monitor human health.

关键词： Multiplexed microfilament electrode cluster Physiological ion sensing Subcutaneous and brain experiment Wearable platform for multi-ion detection Continuous real-time monitoring system

Photoinduced Radical-Ionic Transfer of Various Chlorofluorocarbons to Alkenes from Oxime-Based Surrogates

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CCS Chemistry 2024年第5期6卷 1222-1230页

作者： Jinghui Zhang Muliang Zhang Martin Oestreich Institut für Chemie Technische Universität Berlin10623 Berlin Hefei National Laboratory for Physical sciences at the Microscale and Department of Chemistry University of Science and Technology of ChinaHefei 230026

Functional-group-transfer strategies that avoid the use of unsustainable chemicals are attractive for the development of green ***(CFCs)not only contribute to the depletion of the stratospheric ozone layer,but their gaseous nature also poses a serious threat in scientific ***,the design of effective and sustainable alternatives to CFCs is highly ***,a practical CFC transfer platform for the addition of both a fluoroalkyl group and a chlorine substituent across alkenes by a photomediated redox-neutral manifold using bench-stable and easy-to-handle oxime-based surrogates is *** distinct reactivity of these tunable reagents allows for their single-electron reduction to trigger fragmentation driven by benzonitrile formation and loss of carbon *** other fragments released in that step,namely an electrophilic fluoroalkyl radical and a nucleophilic chloride anion,are subsequently transferred onto alkenes by a radical-ionic mechanism to deliver the desired chlorofluorocarbon products.

关键词： alkenes chlorofluorocarbons functionalgroup transfer radical-ionic crossover photoredox catalysis

Solar-powered methanol synthesis from COhydrogenation with high conversion and selectivity

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science china Chemistry 2024年

作者： Lingzhen Zeng Yongfang Sun Tingting Wang Zeyan Cen Maolin Wang Oriol Angurell Meng Wang Ding Ma Beijing National Laboratory for Molecular sciences New Cornerstone Science LaboratoryCollege of Chemistry and Molecular EngineeringPeking University Leitat Managing Technologies Parc Cientific de BarcelonaEdifici Clúster IIPlanta 4Carrer Baldiri Reixac

Methanol synthesis via CO2hydrogenation stands as a pivotal avenue for CO2conversion and fixation,garnering extensive *** reactor configurations and energy supplies,alongside a spectrum of catalyst formulations,have been developed to enhance reaction metrics including conversion,selectivity,productivity,and *** state-of-the-art Cu-based catalysts from thermal catalysis into a photothermal reactor yielded notable results,achieving an overall CO2conversion of 98%and methanol selectivity of 86%.Utilizing the liquid out/gas in concept （LOGIC） reactor,in which only the catalyst bed is irradiated to raise its temperature,facilitated the condensation of products （H2O and CH3OH）,due to their low vapor *** lower concentration of products in vapor phases ensured the continuous progress of the *** synergistic integration of reactor design and catalyst fabrication could capitalize on the strengths of both components and lead to enhanced performance in methanol synthesis.

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Medicinal chemistry strategies towards the development of non-covalent SARS-CoV-2 Mpro inhibitors

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Acta Pharmaceutica Sinica B 2024年第1期14卷 87-109页

作者： Letian Song Shenghua Gao Bing Ye Mianling Yang Yusen Cheng Dongwei Kang Fan Yi Jin-Peng Sun Luis Menéndez-Arias Johan Neyts Xinyong Liu Peng Zhan Department of Medicinal Chemistry Key Laboratory of Chemical Biology(Ministry of Education)School of Pharmaceutical SciencesCheeloo College of MedicineShandong UniversityJinan 250012China Shenzhen Research Institute of Shandong University Shenzhen 518057China The Key Laboratory of Infection and Immunity of Shandong Province Department of PharmacologySchool of Basic Medical SciencesShandong UniversityJinan 250012China Key Laboratory Experimental Teratology of the Ministry of Education Department of Biochemistry and Molecular BiologySchool of Basic Medical SciencesCheeloo College of MedicineShandong UniversityJinan 250012China Centro de Biologı´a Molecular“Severo Ochoa”(Consejo Superior de Investigaciones Cientı´ficas&Autonomous University of Madrid) Madrid 28049Spain KU Leuven Department of Microbiology and ImmunologyRega Institute for Medical ResearchLaboratory of Virology and ChemotherapyLeuven 3000Belgium

The main protease(M^(pro))of SARS-CoV-2 is an attractive target in anti-COVID-19 therapy for its high conservation and major role in the virus life *** covalent M^(pro)inhibitor nirmatrelvir(in combination with ritonavir,a pharmacokinetic enhancer)and the non-covalent inhibitor ensitrelvir have shown efficacy in clinical trials and have been approved for therapeutic *** antiviral drugs are needed to fight the pandemic,while non-covalent M^(pro)inhibitors could be promising alternatives due to their high selectivity and favorable *** non-covalent M^(pro)inhibitors with desirable properties have been developed based on available crystal structures of M^(pro).In this article,we describe medicinal chemistry strategies applied for the discovery and optimization of non-covalent M^(pro)inhibitors,followed by a general overview and critical analysis of the available *** viewpoints and insights into current strategies for the development of non-covalent M^(pro)inhibitors are also discussed.

关键词： COVID-19 SARS-CoV-2 Main protease Non-covalent inhibitors Medicinal chemistry strategies

The evolving roles of Wnt signaling in stem cell proliferation and differentiation, the development of human diseases, and therapeutic opportunities

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Genes & Diseases 2024年第3期11卷 155-187页

作者： Michael Yu Kevin Qin Jiaming Fan Guozhi Zhao Piao Zhao Wei Zeng Connie Chen Annie Wang Yonghui Wang jiamin Zhong Yi Zhu William Wagstaff Rex C.Haydon Hue H.Luu Sherwin Ho Michael J.Lee Jason Strelzow Russell R.Reid Tong-Chuan He School of Medicine Rosalind Franklin University of Medicine and ScienceNorth ChicagoIL 60064USA Molecular Oncology Laboratory Department of Orthopedic Surgery and Rehabilitation MedicineThe University of Chicago Medical CenterChicagoIL 60637USA Ministry of Education Key Laboratory of Diagnostic Medicine and Department of Clinical BiochemistryThe School of Laboratory MedicineChongqing Medical UniversityChongqing 400016China Department of Orthopedic Surgery The First Affliated Hospital of Chongqing Medical UniversityChongqing 400016China Department of Urology The First Affiliated Hospital of Chongqing Medical UniversityChongqing 400016China Department of Clinical Laboratory Medicine Shanghai Jiaotong University School of MedicineShanghai 200000China Department of Orthopaedic Surgery Chinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing 100730China Laboratory of Craniofacial Suture Biology and Development Department of Surgery Section of Plastic SurgeryThe University of Chicago Medical CenterChicagoIL 60637USA Department of Neurology The First Dongguan Affiliated HospitalGuangdong Medical UniversityDongguanGuangdong 523475China

The evolutionarily conserved Wnt signaling pathway plays a central role in develop-ment and adult tissue homeostasis across *** proteins are secreted,lipid-modified signaling molecules that activate the canonical(β-catenin dependent)and non-canonical(β-catenin independent)Wnt signaling *** behaviors such as proliferation,differ-entiation,maturation,and proper body-axis specification are carried out by the canonical pathway,which is the best characterized of the known Wnt signaling *** signaling has emerged as an important factor in stem cell biology and is known to affect the self-renewal of stem cells in various *** includes but is not limited to embryonic,hematopoietic,mesenchymal,gut,neural,and epidermal stem *** signaling has also been implicated in tumor cells that exhibit stem cell-like *** signaling is crucial for bone formation and presents a potential target for the development of therapeutics for bone *** surprisingly,aberrant Wnt signaling is also associated with a wide variety of diseases,including *** of Wnt pathway members in cancer can lead to unchecked cell proliferation,epithelial-mesenchymal transition,and ***,advances in the understand-ing of dysregulated Wnt signaling in disease have paved the way for the development of novel therapeutics that target components of the Wnt *** with a brief overview of the mechanisms of canonical and non-canonical Wnt,this review aims to summarize the cur-rent knowledge of Wnt signaling in stem cells,aberrations to the Wnt pathway associated with diseases,and novel therapeutics targeting the Wnt pathway in preclinical and clinical studies.

关键词： β-Catenin Cancer Canonical Wnt Disease Non-canonical Wnt Stem cells Targeted therapy Wnt signaling

Highly ordered inkjet-printed quantum-dot thin films enable efficient and stable QLEDs with EQE exceeding 23%

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escience 2024年第3期4卷 152-162页

作者： Changting Wei Bo Xu Meng Zhang Zhenhuang Su Jiawei Gu Wenrui Guo Xingyu Gao Wenming Su Zheng Cui Seokwoo Jeon Zhiyong Fan Haibo Zeng MIIT Key Laboratory of Advanced Display Materials and Devices Institute of Optoelectronics&NanomaterialsSchool of Materials Science and EngineeringNanjing University of Science and TechnologyNanjing 210094China Ningbo Nato New Material Technology Co. LtdNingbo 315600China Shanghai Synchrotron Radiation Facility(SSRF) Zhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China School of Mechanical Engineering Jiangsu UniversityZhenjiang 212013China Printable Electronics Research Center Nano Devices and Materials DivisionSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China Department of Materials science and Engineering Korea UniversitySeoul 02841South Korea Department of Electronic and Computer Engineering The Hong Kong University of Science and TechnologyHong Kong 999077China

Inkjet-printed quantum dot light-emitting diodes(QLEDs)are emerging as a promising technology for next-generation ***,the progress in fabricating QLEDs using inkjet printing technique has been slower compared to spin-coated devices,particularly in terms of efficiency and *** key to achieving high performance QLEDs lies in creating a highly ordered and uniform inkjet-printed quantum dot(QD)thin *** this study,we present a highly effective strategy to significantly improve the quality of inkjet-printed CdZnSe/CdZnS/ZnS QD thin films through a pressure-assisted thermal annealing(PTA)*** from this PTA process,a high quality QD thin film with ordered packing,low surface roughness,high photoluminescence and excellent electrical property is *** mechanism behind the PTA process and its profound impact on device performance have been thoroughly investigated and ***,a record high external quantum efficiency(EQE)of 23.08%with an impressive operational lifetime(T50)of up to 343,342h@100cdm−2,and a record EQE of 22.43%with T50 exceeding to 1,500,463h@100cdm−2 are achieved in inkjet-printed red and green CdZnSe-based QLEDs,*** work highlights the PTA process as an important approach to realize highly efficient and stable inkjet-printed QLEDs,thus advancing QLED technology to practical applications.

关键词： Inkjet printing Quantum dot light-emitting diode High efficiency Thermal annealing Highly ordered