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Hydrogen self-supplying initiators excited by visible light for the fabrication of transparent films

science China Chemistry 2024年第11期67卷 3868-3874页

作者： Qingze Pan Chiheng Liu Wenzhe Qiao Jianwei Li Saihe Yang Yangyang Xin Pengzhong Chen Jiangli Fan Xiaojun Peng State Key Laboratory of Fine Chemicals Frontiers Science Center for Smart Materials Oriented Chemical EngineeringDalian University of TechnologyDalian 116024China Ningbo Institute of Dalian University of Technology Ningbo 315016China Key Lab of Organic Optoelectronics and Molecular Engineering of Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China Liaoning Binhai Laboratory Dalian 116023China

Unimolecular Type Ⅱ radical photoinitiators(PIs) have received significant attention in photocuring owing to the fact that they improve the sustainability of the overall process compared with traditional Type Ⅱ radical photoinitiators. However, the photopolymerization efficiency of unimolecular Type Ⅱ radical photoinitiators is hindered by their short excitation wavelengths,poor photon capture abilities, and inefficient photobleaching performance. Herein, we report a coumarin-based self-sufficient initiator(C-NA), which is designed by integrating “hydrogen donor” and “hydrogen acceptor” into the coumarin framework and used for single-component visible light curing. C-NA exhibits a visible light absorbance and high molar extinction coefficient and is completely photobleached under the irradiation of 405 nm light-emitting diodes(LEDs). The formation of free radicals arises from the transfer of hydrogen from the diethylamino group to the coumarin framework, together with a highly efficient photodegradation process of C-NA. Finally, C-NA was successfully applied to prepare a transparent film material. Therefore,C-NA offers new insights into the design of promising unimolecular Type Ⅱ radical photoinitiators for photocuring.

关键词： photocuring photoinitiator hydrogen transfer visible light unimolecular photobleaching

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Special issue on “Green chemical process and intensification”

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Frontiers of chemical science and engineering 2022年第11期16卷 1533-1535页

作者： You Han Xiang Ma Lin-Bing Sun Jianhong Xu School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China Key Laboratory for Advanced Materials and Institute of Fine Chemicals School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Material(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China The State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

In order to better unite and lead young chemical engineering scholars,the chemical Industry and engineering Society of China will establish Youth Working *** the time of the establishment of Youth Working Committee,we were invited as guest editors to organize the special issue of Frontiers of chemical science and engineering on green chemical process and intensification,aiming to inspire the innovative ideas and build an energetic and academic communication platform for young scholars.

关键词： intensification process chemical

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Local-strain-induced CO2 adsorption geometries and electrochemical reduction pathway shift

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National science Review 2024年第12期11卷 20-27页

作者： Chuhao Liu Yifan Bu Yifei Xu Azhar Mahmood Jisheng Xie Yifan Fu Shiyun Li Cheng Peng Yue Wu Xiao Liang Ruilong Zong Wan-Lu Li Jihan Zhou Bingjun Xu Li Niu Mufan Li College of Chemistry and Molecular Engineering Peking University School of Chemistry and Chemical Engineering Guangzhou University College of Materials Science and Engineering Fuzhou University Department of Chemistry Tsinghua University Department of Nano Engineering University of California

Unravelling the influence of strain and geometric effects on the electrochemical reduction of carbon dioxide（CO2RR） on Cu-based（or Pd-based） alloys remains challenging due to complex local microenvironment variables. Herein, we employ two Pd Cu alloys（nanoparticles and nanodendrites） to demonstrate how CO2RR selectivity can shift from CO to HCOO-. Despite sharing consistent phases, exposed crystal facets,and overall oxidative states, these alloys exhibit different local strain profiles due to their distinct *** integrating experimental data, in-situ spectroscopy, and density functional theory calculations, we revealed that CO2prefers adsorption on tensile-strained areas with carbon-side geometry, following a*COOH-to-CO pathway. Conversely, on some compressive-strained regions induced by the dendrite-like morphology, CO2adopts an oxygen-side geometry, favoring an *OCHO-to-HCOO pathway due to the downshift of the d-band center. Notably, our findings elucidate a dominant *OCHO-to-HCOO-pathway in catalysts when featuring both adsorption geometries. This research provides a comprehensive model for local environment of bimetallic alloys, and establishes a clear relationship between the CO2RR pathway shift and variation in local strain environments of PdCu alloys.

关键词： local strain CO electroreduction pathway shift PdCu alloys

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Continuous Lithium-Ion Extraction From Seawater and Mine Water With a Fuel Cell System and Ceramic Membranes

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Energy & Environmental materials 2024年第6期 258-265页

作者： Cansu K?k Lei Wang Jean Gustavo A.Ruthes Antje Quade Matthew E.Suss Volker Presser INM-Leibniz Institute for New Materials Department of Materials Science & Engineering Saarland University Leibniz Institute for Plasma Science and Technology Faculty of Mechanical Engineering Technion-Israel Institute of Technology Wolfson Department of Chemical Engineering Technion-Israel Institute of Technology Grand Technion Energy Program Technion-Israel Institute of Technology Saarene-Saarland Center for Energy Materials and Sustainability

The demand for electronic devices that utilize lithium is steadily increasing in this rapidly advancing technological *** high-purity lithium in an environmentally friendly way is challenging by using commercialized ***,we propose the first fuel cell system for continuous lithium-ion extraction using a lithium superionic conductor membrane and advanced *** fuel cell system for extracting lithium-ion has demonstrated a twofold increase in the selectivity of Li+/Na+while producing electricity.

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Organic X-Ray Image Sensors Using a Medium Bandgap Polymer Donor with Low Dark Current

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Energy & Environmental materials 2024年第6期7卷 230-237页

作者： Jong-Woon Ha Seung Hun Eom Bo Kyung Cha Seyeong Song Hyeong Ju Eun Jong H.Kim Jong Mok Park BongSoo Kim Byoungwook Park Seo-Jin Ko Sung Cheol Yoon Changjin Lee In Hwan Jung Do-Hoon Hwang Department of Chemistry Chemistry Institute for Functional MaterialsPusan National UniversityBusan 46241Korea Division of Advanced Energy Materials Research Center Korea Research Institute of Chemical Technology(KRICT)Daejeon 34114Korea Electro-Medical Device Research Center Korea Electrotechnology Research Institute(KERI)Ansan 15588Korea Graduate School of Carbon Neutrality School of Energy and Chemical EngineeringUlsan National Institute of Science and Technology(UNIST)Ulsan 44919Korea Department of Molecular Science and Technology Ajou UniversitySuwon 16449Korea Research Center for Advanced Specialty Chemicals Korea Research Institute of Chemical TechnologyUlsan 44412Korea Department of Chemistry Ulsan National Institute of Science and Technology(UNIST)Ulsan 44919Korea Department of Organic and Nano Engineering Human-Tech Convergence ProgramHanyang University222 Wangsimni-roSeongdong-guSeoul 04763Korea

The development of portable X-ray detectors is necessary for diagnosing fractures in unconscious patients in emergency ***,this is quite challenging because of the heavy weight of the scintillator and silicon *** weight and thickness of X-ray detectors can be reduced by replacing the silicon layer with an organic *** study presents a novel bithienopyrroledione-based polymer donor that exhibits excellent photodetection properties even in a thick photoactive layer(~700 nm),owing to the symmetric backbone and highly soluble molecular structure of *** ability of bithienopyrroledione-based polymer donor to strongly suppress the dark current density(Jd~10−10 A cm^(−2))at a negative bias(−2.0 V)while maintaining high responsivity(R=0.29 A W−1)even at a thickness of 700 nm results in a maximum shot-noise-limited specific detectivity of D_(sh)^(*)=2.18×10^(13)Jones in the organic *** organic photodetectors are developed by slot-die coating for use in X-ray detectors,which exhibit D_(sh)^(*)=2.73×10^(12)Jones with clear rising(0.26 s)and falling(0.29 s)response times upon X-ray *** reliability is also proven by linear response of the X-ray detector,and the X-ray detection limit is 3 mA.

关键词： low dark current low detection limit organic photodetector printable X-ray

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Unraveling the relationship between Sr stoichiometry in Sr_(x)Fe_(1.5)Mo_(0.5)O_(6)-σ and its catalytic performance for high-temperature CO_(2) electrolysis

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materials Reports(Energy) 2023年第1期3卷 86-92,I0003页

作者： Xiuan Xi Xiaoyu Liu Lingui Huang Jianwen Liu Bo-Wen Zhang Gadi Rothenberg Xian-Zhu Fu Jing-Li Luo College of Materials Science and Engineering Shenzhen UniversityShenzhen518060China Department of Chemical and Materials Engineering University of AlbertaEdmontonABT6G 1H9Canada Van‘t Hoff Institute for Molecular Sciences University of AmsterdamScience Park 9041098XHAmsterdamthe Netherlands

The solid oxide electrolytic cell(SOEC)is one of the most promising energy conversion and storage devices,which could convert CO_(2) to CO with high Faradaic efficiency and production ***,the lack of active and stable cathode materials impedes their practical *** we focus on the promising perovskite oxide cathode material Sr_(2)Fe_(1.5)Mo_(0.5)O_(6)-σ,with the aim of understanding how A-atom stoichiometry and catalytic performance are *** find that increasing the strontium content in the perovskite improves the chemisorption of CO_(2) on its surface,forming a SrCO_(3) *** hinders the charge transfer and oxygen exchange ***-neously,strontoium segregation to the cathode surface facilitates coking of the surface during CO_(2) electrolysis,which poisons the ***,a small number of Sr deficiencies are optimal for both electrochemical performance and long-term *** results provide new insights for designing high-performance CO_(2) electrolysis cathode materials.

关键词： SOECs Perovskite oxides Cathode Sr segregation CO_(2) electrolysis

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Organic stoichiometric cocrystals with a subtle balance of charge-transfer degree and molecular stacking towards high-efficiency NIR photothermal conversion

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Chinese chemical Letters 2024年第10期35卷 180-186页

作者： Jieqiong Xu Wenbin Chen Shengkai Li Qian Chen Tao Wang Yadong Shi Shengyong Deng Mingde Li Peifa Wei Zhuo Chen Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui Graphene Engineering LaboratoryAnhui UniversityHefei 230601China Molecular Science and Biomedicine Laboratory(MBL).State Key Laboratory of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringCollege of BiologyAptamer Engineering Center of Hunan ProvinceHunan UniversityChangsha 410082China Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou UniversityShantou515063China

Charge-transfer(CT)stoichiometric cocrystals are promising choice of organic materials for unveiling the structure-property ***,due to the contradiction between large CT degree required for strong NIR absorption and flexible molecular stacking,construction of stoichiomorphism-based cocystals with near-infrared(NIR)photothermal property remains ***,the first example of stoichiomorphism-based photothermal cocrystals were accomplished through the adaptive assembly of 3,3,5,5-tetramethylbenzidine(TMB)donor and 1,2,4,5-tetracyanobenzene(TCNB)*** selective cocrystallization could be controlled by varying the donor-acceptor stoichiometries via a surfactantassisted method,resulting in two cocrystals with 1:1(T1C1)and 1:2(T2C1)*** absorbance intensity of T1C1 at 808 nm was nearly twice that of T2C1,while the photothermal conversion efficiency(PCE)of the former was 60.3%±0.6%,approximately 80%of that for the latter(75.5%±2.6%),which might be caused by the different intermolecular interactions in distinct molecular stacking ***,both excellent PCEs of stoichiometric cocrystals were attributed to the nonradiative transition process,including internal conversion and charge dissociation processes,as elucidated by femtosecond transient absorption spectroscopy ***,T1C1 was used as an NIR heater for preparing agarose-based photothermal hydrogel,showing great potential for light-controlled in-situ *** strategy of balancing the CT degree and molecular packing orientation not only uncovered the relationship between stoichiometric stacking and photothermal property,but also provided an opportunity to develop advanced organic optoelectronic materials.

关键词： Charge-transfer cocrystal Stoichiometric stacking Crystal growth Photothermal conversion In-situ gelation

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A rechargeable and portable hydrogen storage system grounded on soda water

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Chinese chemical Letters 2025年第3期36卷 305-310页

作者： Lingyun Shen Shenxiang Yin Qingshu Zheng Zheming Sun Wei Wang Tao Tu State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering School of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021China Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China Frontiers Science Center for Transformative Molecules Shanghai Key Laboratory for Molecular Engineering of Chiral DrugsSchool of Chemistry and Chemical Engineering and Zhangjiang Institute for Advanced StudyShanghai Jiao Tong UniversityShanghai 200240China Departments of Pharmacology and Toxicology and Chemistry and Biochemistry University of ArizonaTucsonAZ 85721United States State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

The bicarbonate-formate(HCO_(3)−–HCO_(2)−)interconversion provides a promising cycle for a conveniently accessible hydrogen storage system via reversible dehydrogenation and hydrogenation *** catalytic systems often use organic solvents,tedious optimization as well as manipulation of pH values,solvent,pressure and various ***,we present an operational,robust,safe and cost-effective catalytic system for hydrogen storage and *** have established a unique catalytic system with two different solid organometallic assemblies(NHC-Ru and NHC-Ir)that facilitate the reversible transformation between sodium formate and bicarbonate in aqueous solutions collaboratively and ***,the NHC-Ru catalyst is privileged for the hydrogenation of sodium bicarbonate,whereas the NHC-Ir component enables the dehydrogenation of sodium formate,all in a single reaction *** sets this system apart is its *** H_(2)discharging and recharging is simply regulated by heating the mixture with or without H_(2).Remarkably,this process requires no extra additives or supplementary ***,the reversible hydrogen storage system is durable and can be reused for over 30 cycles without a discernible decline in activity and *** strategic paradigm in this study shows significant practical potential in hydrogen fuel cell applications.

关键词： Dehydrogenation Hydrogen storage Hydrogenation N-Heterocyclic carbene Soda water

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Facile synthesis of azobenzene-embedded conjugated macrocycles for optically switchable single-crystal transistors and tunable supramolecular assemblies

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Aggregate 2023年第6期4卷 101-109页

作者： Dongdong Chang Xuetao Xiao Dongyue An Rong Zhang Xianyu Song Yunqi Liu Yan Zhao Xuefeng Lu Department of Materials Science State Key Laboratory of Molecular Engineering of PolymersFudan UniversityShanghaiChina Key Laboratory of Water Environment Evolution and Pollution Control in Three Gorges Reservoir School of Environmental and Chemical EngineeringChongqing Three Gorges UniversityChongqingChina

A series of newπ-conjugated macrocycles(AzoM-n-E,n 1–3)incorporating=azobenzene units have been synthesized by a facile strategy in one-pot *** resultant azobenzene-embedded macrocycles feature intrinsic photoresponsive behaviors and intriguing supramolecular assembling *** smallest macro-cycle AzoM-1-E with a rigid planar conjugated backbone structure is used to prepare the single crystal transistors,showing reversible optical *** moderate size macrocycle AzoM-2-E assembles into a dimer in the form of interpenetration throughπ-πstacking between azobenzene *** largest macrocycle AzoM-3-E with enhancedﬂexibility can adaptively assemble with various types of electron-deﬁcient guests accompanied by distortion of ***,AzoM-3-E assembles with the planar F4-TCNQ to form a tetragonal geometry by C-F⋅⋅⋅π and π-π interactions,while the assembly with ellipsoidal C70 viaπ-πinteractions induces AzoM-3-E to form a boat-shaped *** work will shed new light on the development of functional conjugated macrocycles in organic electronics.

关键词： azobenzene conjugated macrocycle host-guest interaction photoresponsive transistors supramolecular assembly

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Bipolar Thermally Activated Delayed Fluorescence Emitter with Balanced Carrier Transport for High-Efficiency Nondoped Green Electroluminescent Devices

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CCS Chemistry 2024年第9期6卷 2346-2357页

作者： Yuchao Liu Zhagen Miao Haikuo Gao Shian Ying Can Gao Shouke Yan Huanli Dong Zhongjie Ren Key Laboratory of Rubber-Plastics Ministry of Education/Shandong Provincial Key Laboratory of Rubber-PlasticsSchool of Polymer Science and EngineeringQingdao University of Science and TechnologyQingdao 266042 National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Department of Chemistry University of Chinese Academy of SciencesBeijing 100049 Shandong Engineering Research Center of Aeronautical Materials and Devices College of Aeronautical EngineeringBinzhou UniversityBinzhou 251900 State Key Laboratory of Chemical Resource Engineering College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029

High-efficiency electroluminescent devices featuring simplified architecture have received considerable attention due to significant advantages in construction procedures and commercialized ***,there still remains a critical challenge with regard to the lack of organic semiconductors that simultaneously possess high luminescent efficiency and balanced carrier-transporting ***,we design a thermally activated delayed fluorescence(TADF)emitter 4-(9,9-dimethyl-9,10-dihydroacridine)-4′-triphenylphosphineoxide-benzophenone(DMAC-BPTPO)by incorporating triphenylphosphine oxide into the donor–acceptor *** accessional electrontransporting moiety,rod-like dimer,and horizontally packing model synergistically enable DMAC-BP-TPO which possesses an excellent photoluminescence quantum yield of nearly 90%with a reverse intersystem crossing rate constant of 2.0×106 s−1,horizontal dipole ratio of 89%,and a balanced electron and hole mobilities with a small constrast ratio of ***,simplified electroluminescent devices including organic lightemitting diodes(OLEDs)and organic light-emitting transistors(OLETs)incorporating DMAC-BP-TPO-based nondoped film are demonstrated due to their superior integrated optoelectronic properties along with preferable horizontal dipole orientation.A record-high external quantum efficiency value of 21.7%and 4.4%are finally achieved in the simplified nondoped OLED and OLET devices,which are among the highest values in the related research *** work provides a new avenue to develop a high-efficiency bipolar TADF emitter to advance the simplified electroluminescent devices.

关键词： organic light-emitting diode organic lightemitting transistor bipolar thermally activated delayed fluorescence nondoped active layer

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