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

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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 Engineering Dalian University of Technology Ningbo Institute of Dalian University of Technology key lab of organic optoelectronics and molecular engineering of ministry of education Department of Chemistry Tsinghua University Liaoning Binhai laboratory

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

Structural transformation from Waugh-type to Keggin-type polyoxomolybdate-based crystalline material for photo/electrocatalysis

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Rare Metals 2024年第5期43卷 2241-2250页

作者： Pei-Sen Wang Zi-Tong Wang Ya-Ya Tan Peng Chen Xue-Cheng Zhang Lu-Nan Zhang Yong-Ge Wei Lu-Bin Ni School of Chemistry and Chemical engineering Yangzhou UniversityYangzhou 225002China key lab of organic optoelectronics and molecular engineering of ministry of education Department of ChemistryTsinghua UniversityBeijing 100084China State key laboratory of Natural and Biomimetic Drugs Peking UniversityBeijing100191China

An inorganicDorganic hybrid crystalline material(SiMo_(12)O_(40))[Cu(2,2'-bipy)_(2)]_(2)·2H_(2)O(Complex 1,2,2'-bipy=2,2'-bipyridine)was synthesized for the first time by using 2,2'-bipy and transition metal copper to convert Waugh-type polyoxometalate[MnMo_(9)O_(3)_(2)]_(6-)into a Keggin polyoxometalate structure[SiMo_(12)O_(40)]^(4-)under hydrothermal conditions in glass *** crystal tests and a series of characterizations were carried out on Complex *** structure of Complex 1 is composed of[SiMo_(12)O_(40)]^(4-)and[Cu^(Ⅱ)(2,2'-bipy)_(2)]^(2+).The five-coordinated Cu is connected to two 2,2'-bipy through CuDN bonds,forming an approximately square ***,Complex 1 exhibited good photocatalytic performance for methylene blue degradation and electrocatalytic nitrite reduction properties simultaneously.

关键词： Polyoxometalates Inorganic-organic hybrid materials Photocatalytic Electrocatalytic

Promising thermal photonic management materials for sustainable human habitat

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Nano Research 2024年第1期17卷 112-131页

作者： Houze Yao Qihua Liao Huhu Cheng Liangti Qu key laboratory of organic optoelectronics&molecular engineering Ministry of EducationDepartment of ChemistryLaboratory of Flexible Electronics TechnologyTsinghua UniversityBeijing 100084China State key laboratory of Tribology in Advanced Equipment(SKLT) Department of Mechanical EngineeringTsinghua UniversityBeijing 100084China

The spectral characteristics of outdoor structures,such as automobiles,buildings,and clothing,determine their energy interaction with the environment,from broad-spectrum absorption of light energy to high-efficiency thermal *** developed spectrally selective absorption(SSA)materials permit the reduction of energy loss from human habitat eco-system in the sustainable way and further reduce the utilization of fossil energy to achieve carbon *** we review recent advances in SSA materials that enable rational and efficient management of thermal energy and provide new solutions for the resource base that supports human life like comfortable heat management,electricity production,and water *** basic principles of thermal photonic management,the regulation of SSA materials,and functional properties are *** outlook discussing challenges and opportunities in SSA material energy management for comfortable living environments is finally presented,which expects the enormous potential of this interdisciplinary research in solving growing resource-shortage of human society.

关键词： spectrally selective absorption passive cooling solar power eco-system

Polymer: Non-fullerene acceptor heterojunction-based phototransistor for short-wave infrared photodetection

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Nano Research 2024年第4期17卷 3087-3095页

作者： Jing Li Weigang Zhu Yang Han Yanhou Geng Wenping Hu key laboratory of organic Integrated Circuits of ministry of education&key laboratory of molecular Optoelectronic Sciences School of Science&Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300072China key laboratory of organic Integrated Circuits of ministry of education&key laboratory of molecular Optoelectronic Sciences School of Materials Science and EngineeringTianjin UniversityTianjin 300072China

It remains full of challenge for extending short-wave infrared(SWIR)spectral response and weak-light detection in the context of broad spectral responses for *** this work,a novel poly(2,5-bis(4-hexyldodecyl)-2,5-dihydro-3,6-di-2-thienyl-pyrrolo[3,4-c]pyrrole-1,4-dione-alt-thiophene)(PDPPT3-HDO):COTIC-4F organic bulk-heterojunction is prepared as active layer for bulk heterojunction ***3-HDO serves as a hole transport material,while COTIC-4F enhances the absorption of SWIR light to 1020 *** a result,smooth and connected PDPPT3-HDO film is fabricated by blade coating method and exhibits high hole mobility up to 2.34 cm^(2)·V^(-1)·s^(-1) with a current on/off ratio of 4.72×10^(5) in organic thin film ***3-HDO:COTIC-4F heterojunction phototransistors exhibit high responsivity of 2680 A·W^(-1) to 900 nm and 815 A·W^(-1) to 1020 nm,with fast response time(rise time~20 ms and fall time~100 ms).The photosensitivity of the heterojunction phototransistor improves as the mass ratio of non-fullerene acceptors increases,resulting in an approximately two orders of magnitude enhancement compared to the bare polymer ***,the phototransistor exhibits decent responsivity even under ultra-weak light power of 43μW·cm^(-2) to 1020 *** work represents a highly effective and general strategy for fabricating efficient and sensitive SWIR light photodetectors.

关键词： photodetection phototransistor organic semiconductor heterojunction non-fullerene acceptor

Revolutionizing wearable healthcare with solid-state epidermal biomarker monitoring

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Science Bulletin 2024年第17期69卷 2650-2652页

作者： Huarun Liang Yingying Zhang key laboratory of organic optoelectronics and molecular engineering of ministry of education Department of ChemistryTsinghua UniversityBeijing 100084China

In modern medical research, the analysis of biomarkers in biofluids such as blood, urine, saliva, and sweat is indispensable for revealing human physiological processes and disease states[1-4]. However, existing detection methods face significant challenges. Blood and urine analyses are not only inconvenient and costly but also struggle to achieve continuous monitoring. Saliva analysis can be compromised by food residues and bacteria. Additionally, the long-term use of sweat-inducing drugs or iontophoresis [5], aimed at enabling continuous monitoring of biomarkers in sweat for sedentary individuals, may result in discomfort and side effects [6,7].

关键词： urine Blood wear

Peripheral carbazole units-decorated MR emitter containing B−N covalent bond for highly efficient green OLEDs with low roll-off

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Journal of Semiconductors 2024年第8期45卷 59-66页

作者： Danrui Wan Jianping Zhou Guoyun Meng Ning Su Dongdong Zhang Lian Duan Junqiao Ding School of Chemical Science and Technology Yunnan UniversityKunming 650091China key laboratory of organic optoelectronics and molecular engineering of ministry of education Department of ChemistryTsinghua UniversityBeijing 100084China Southwest United Graduate School Kunming 650092China

Boron−nitrogen doped multiple resonance(BN-MR)emitters,characterized by B−N covalent bonds,offer distinctive advantages as pivotal building blocks for facile access to novel MR emitters featuring narrowband spectra and high ***,there remains a scarcity of exploration concerning synthetic methods and structural derivations to expand the library of novel BN-MR ***,we present the synthesis of a BN-MR emitter,tCz[B−N]N,through a one-pot borylation reaction directed by the amine group,achieving an impressive yield of 94%.The emitter is decorated by incorporating two 3,6-di-tbutylcarbazole(tCz)units into a B−N covalent bond doped BN-MR parent molecule via para-C−π−D and para-N−π−D *** peripheral decoration strategy enhances the reverse intersystem crossing process and shifts the emission band towards the pure green region,peaking at 526 nm with a narrowband full-width at half maximum(FWHM)of 41 ***,organic light emitting diodes(OLEDs)employing this emitter achieved a maximum external quantum efficiency(EQEmax)value of 27.7%,with minimal efficiency *** at a practical luminance of 1000 cd·m^(−2),the device maintains a high EQE value of 24.6%.

关键词： multi-resonance narrowband emission B−N covalent bond organic light emitting diodes

Moisture‑Electric–Moisture‑Sensitive Heterostructure Triggered Proton Hopping for Quality‑Enhancing Moist‑Electric Generator

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Nano-Micro Letters 2024年第3期16卷 351-366页

作者： Ya’nan Yang Jiaqi Wang Zhe Wang Changxiang Shao Yuyang Han Ying Wang Xiaoting Liu Xiaotong Sun Liru Wang Yuanyuan Li Qiang Guo Wenpeng Wu Nan Chen Liangti Qu key laboratory of Cluster Science Ministry of Education of ChinaKey Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China Yangtze Delta Region Academy of Beijing Institute of Technology Jiaxing 314019People’s Republic of China Department of Chemistry Key Laboratory of Organic Optoelectronics&Molecular EngineeringMinistry of EducationTsinghua UniversityBeijing 100084People’s Republic of China

Moisture-enabled electricity(ME)is a method of converting the potential energy of water in the external environment into electrical energy through the interaction of functional materials with water molecules and can be directly applied to energy harvesting and signal ***,ME can be unreliable in numerous applications due to its sluggish response to moisture,thus sacrificing the value of fast energy harvesting and highly accurate information ***,by constructing a moisture-electric-moisture-sensitive(ME-MS)heterostructure,we develop an efficient ME generator with ultra-fast electric response to moisture achieved by triggering Grotthuss protons hopping in the sensitized ZnO,which modulates the heterostructure built-in interfacial potential,enables quick response(0.435 s),an unprecedented ultra-fast response rate of 972.4 mV s^(−1),and a durable electrical signal output for 8 h without any *** research provides an efficient way to generate electricity and important insight for a deeper understanding of the mechanisms of moisture-generated carrier migration in ME generator,which has a more comprehensive working scene and can serve as a typical model for human health monitoring and smart medical electronics design.

关键词： Moist-electric generators Grotthuss proton hopping Fast response Durable electrical output Personal health monitoring

Versatile Organogels of Aluminum Oxide Subnanosheets for Locking Solvents and Adhesion

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Precision Chemistry 2024年第1期2卷 21-27页

作者： Wanyue Ouyang Xun Wang key lab of organic optoelectronics and molecular engineering Department of ChemistryTsinghua UniversityBeijing 100084China

Herein,we present a facile strategy to prepare versatile aluminum oxide subnanometer nanosheets with oleic acid and stearic acid ligands(OA-Al SNSs and SA-Al SNSs,respectively).The size effect endows subnanosheets with abundant acting sites,remarkable intermolecular interactions,and unique polymer-like properties,including flexibility,viscoelasticity,and sol-gel transitions,which is quite different from traditional inorganic ***,subnanosheets could form freestanding organogels and OA-Al SNSs exhibit satisfying semisolidification of various solvents,making it an intriguing candidate for the safe storage and transportation of ***,SA-Al SNSs exhibit excellent adhesive properties of high strength on diverse substrates,and it is easy to erase it without any damage,demonstrating the promising prospects in practical applications.

关键词： subnanometer nanomaterials self-assembly polymer-analogue organogel adhesive

Recent progress on the functionalization of white phosphorus in China

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National Science Review 2024年第6期11卷 308-320页

作者： Xinlei Huangfu Zhongzhen Wang Yu Chen Junnian Wei Wei Liu Wen-Xiong Zhang Beijing National laboratory for molecular Sciences(BNLMS) State Key Laboratory of Rare-Earth Materials Chemistry and Applications & Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular Engineering Peking University

Direct synthesis of organophosphorus compounds from white phosphorus represents a significant but challenging subject, especially in the context of ongoing efforts to comprehensively improve the phosphorus-derived chemical industry driven by sustainability and safety concerns. China is the world's largest producer of white phosphorus, creating a significant demand for the green transformation of this crucial feedstock. This review provides an overview of advancements in white phosphorus activation by Chinese research teams, focusing on the direct construction of P–C/N/O/S/M bonds from white phosphorus. Additionally, we offer some insights into prospective directions for the activation and transformation of white phosphorus in the future. This review paper aims to attract more researchers to engage in this area, stimulating follow-up exploration and fostering enduring advances.

关键词： white phosphorus organophosphorus compound activation selectivity efficiency