检索结果-内蒙古大学图书馆

Molecular Engineering of Methylated Sulfone-Based Covalent Organic Frameworks for Back-Reaction Inhibited Photocatalytic Overall Water Splitting

引用

Angewandte Chemie 2024年第37期136卷

作者： Xiang Zhang Zhiwei Xiao Lei Jiao Huyue Wu Yan-Xi Tan Jing Lin Daqiang Yuan Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China College of Chemistry and Materials Science Fujian Normal University Fuzhou 350007 P. R. China

Solar-to-hydrogen (H 2 ) and oxygen (O 2 ) conversion via photocatalytic overall water splitting (OWS) holds great promise for a sustainable fuel economy, but has been challenged by the backward O 2 reduction reaction (ORR) with favored proton-coupled electron transfer (PCET) dynamics. Here, we report that molecular engineering by methylation inhibits the backward ORR of molecular photocatalysts and enables efficient OWS process. As demonstrated by a benchmark sulfone-based covalent organic framework (COF) photocatalyst, the precise methylation of its O 2 adsorption sites effectively blocks electron transfer and increases the barrier for hydrogen intermediate desorption that cooperatively obstructs the PCET process of ORR. Methylation also repels electrons to the neighboring photocatalytic sulfone group that promotes the forward H 2 evolution. The resultant DS-COF achieves an impressive inhibition of about 70 % of the backward reaction and a three-fold enhancement of the OWS performance with a H 2 evolution rate of 124.7 μmol h −1 g −1 , ranking among the highest reported for organic-based photocatalysts. This work provides insights for engineering photocatalysts at the molecular level for efficient solar-to-fuel conversion.

关键词：

来源：评论

学校读者我要写书评

暂无评论

Coupling Electron Transfer and Redox Site in Boranil Covalent Organic Framework Toward Boosting Photocatalytic Water Oxidation

引用

Angewandte Chemie 2024年第13期136卷

作者： Rahul Anil Borse Yan-Xi Tan Jing Lin Enbo Zhou Yangdan Hui Prof. Daqiang Yuan Prof. Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences 350002 Fuzhou Fujian P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China 350108 Fuzhou Fujian P. R. China University of Chinese Academy of Sciences 100049 Beijing P. R. China Institute of Molecular Engineering Plus Fuzhou University 350108 Fuzhou Fujian P. R. China

The efficient polymeric semiconducting photocatalyst for solar-driven sluggish kinetics with multielectron transfer oxygen evolution has spurred scientific interest. However, existing photocatalysts limited by π-conjugations, visible-light harvest, and charge transfer often compromise the O 2 production rate. Herein, we introduced an alternative strategy involving a boranil functionalized-based fully π-conjugated ordered donor and acceptor (D–A) covalent organic frameworks ( Ni-TAPP-COF-BF 2 ) photocatalyst. The co-catalyst-free Ni-TAPP-COF-BF 2 exhibits an excellent ~11-fold photocatalytic water oxidation rate, reaching 1404 μmol g −1 h −1 under visible light irradiation compared to pristine Ni-TAPP-COF (123 μmol g −1 h −1 ) alone and surpasses to reported organic frameworks counterpart. Both experimental and theoretical results demonstrate that the push/pull mechanism (metalloporphyrin/BF 2 ) is responsible for the appropriate light-harvesting properties and extending π-conjugation through chelating BF 2 moieties. This strategy benefits in narrowing band structure, improving photo-induced charge separation, and prolonged charge recombination. Further, the lower spin magnetic moment of M-TAPP-COF-BF 2 and the closer d-band center of metal sites toward the Fermi level lead to a lower energy barrier for *O intermediate. Reveal the potential of the functionalization strategy and opens up an alternative approach for engineering future photocatalysts in energy conversion applications.

关键词： covalent organic frameworks boranil-metalloporphyrin oxygen evolution reaction donor-acceptor-photocatalysts density functional theory

来源：评论

学校读者我要写书评

暂无评论

Lanthanide-doped near-infrared Ⅱ luminescent nanoprobes for bioapplications

引用

Science China Materials 2019年第8期62卷 1071-1086页

作者： Shaohua Yu Datao Tu Wei Lian Jin Xu Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China University of Chinese Academy of Sciences Beijing 100049 China College of Chemistry Fuzhou University Fuzhou 350116 China

Luminescent biosensing in the second nearinfrared(NIR-II) region is featured with superior spatial resolution and high penetration depth by virtue of the suppressed scattering of long-wavelength photons. Hitherto, the reported NIR-II nanoprobes are mostly based on carbon nanotubes, organic fluorophores or semiconducting quantum dots. As an alternative, trivalent lanthanide ions(Ln3+) doped nanoparticles have been emerging as a novel class of promising nanoprobes. In this review, we highlight the recent progress in the design of highly efficient Ln3+-doped NIR-II nanoparticles towards their emerging bioapplications, with an emphasis on autofluorescence-free bioimaging, sensitive bioassay, and accurate temperature sensing. Moreover, some efforts and challenges towards this rapidly expanding field are envisioned.

关键词： lanthanide ions nanoprobe near-infrared Ⅱluminescence bioimaging bioassay temperature sensing

来源：评论

学校读者我要写书评

暂无评论

Fluorinated Polyimide Tunneling Layer for Efficient and Stable Perovskite Photovoltaics

引用

Angewandte Chemie 2024年第21期136卷

作者： Chunming Liu Wei Yu Yuheng Li Can Wang Zilong Zhang Chi Li Lusheng Liang Kangcheng Chen Lin Liu Tinghao Li Xuteng Yu Yao Wang Prof. Peng Gao Institution CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Laboratory for Advanced Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen 361021 China Fujian College University of Chinese Academy of Sciences Fuzhou 350002 China University of Chinese Academy of Sciences Beijing 100049 China College of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 China Instrumentation and Service Center for Physical Sciences Westlake University Hangzhou 310024 China

Despite the remarkable progress of perovskite solar cells (PSCs), challenges remain in terms of finding effective and viable strategies to enhance their long-term stability while maintaining high efficiency. In this study, a new insulating and hydrophobic fluorinated polyimide (FPI: 6FDA-6FAPB) was used as the interface layer between the perovskite layer and the hole transport layer (HTL) in PSCs. The functional groups of FPI play a pivotal role in passivating interface defects within the device. Due to its high work function, FPI demonstrates field-effect passivation (FEP) capabilities as an interface layer, effectively mitigating non-radiative recombination at the interface. Notably, the FPI insulating interface layer does not impede carrier transmission at the interface, which is attributed to the presence of hole tunneling effects. The optimized PSCs achieve an outstanding power conversion efficiency (PCE) of 24.61 % and demonstrate excellent stability, showcasing the efficacy of FPI in enhancing device performance and reliability.

关键词： fluorinated polyimide perovskite solar cells tunneling layer field-effect passivation

来源：评论

学校读者我要写书评

暂无评论

The Marriage of Perovskite Quantum Dots with Rare-Earth Emitters

The Marriage of Perovskite Quantum Dots with Rare-Earth Emit...

引用

中国化学会第十届全国无机化学学术会议

作者： Wei Zheng Zhongliang Gong Datao Tu Ping Huang Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

Perovskite quantum dots(PeQDs) are emerging as a new generation of optoelectronic and photovoltaic materials owing to their outstanding optoelectronic properties such as long carrier diffusion distance, large absorption coefficient, high photoluminescence(PL) quantum yield(QY), narrow emission band, and tunable band gap and PL emission by varying the halide composition.[1,2] The combination of PeQDs with rare-earth(RE) emitters may bring about new optical, electric, thermal, and magnetic properties.[3] In this talk, we shall focus on our recent efforts on the development of PeQDs and RE hybridized materials based on RE-doped PeQDs and PeQDs/RE hetero-structures. Specifically, through sensitization by RE-doped nanoparticles, we have realized full-spectrum photon upconversion tuning in all-inorganic CsPbX3(X = Cl, Br, and I) PeQDs under low power density excitation, with a color gamut of 140% NTSC, upconversion QYs approaching 0.5%, and significantly lengthened exciton lifetimes from μs to ms scale.[4] We have also developed a novel strategy for fine-tuning the persistent luminescence with a color gamut of 130% NTSC and highly synchronized afterglow decay over 8 h by using CsPbX3 PeQDs as efficient afterglow light conversion materials.[5] These findings provide a general approach for tailoring the upconversion and persistent luminescence by the marriage of PeQDs with RE emitters, thereby opening up new opportunities for PeQDs and RE emitters towards many emerging applications such as solar spectrum conversion, white-emitting persistent light source, complex data storage, and multilevel anti-counterfeiting.

关键词： perovskite quantum dots rare earths energy transfer upconversion luminescence persistent luminescence

来源：评论

学校读者我要写书评

暂无评论

The Marriage of Perovskite Quantum Dots with Rare-Earth Emitters

The Marriage of Perovskite Quantum Dots with Rare-Earth Emit...

引用

第九届国际稀土开发与应用研讨会暨2019中国稀土学会学术年会

作者： Wei ZHENG Zhongliang GONG Datao TU Ping HUANG Xueyuan CHEN CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences

Perovskite quantum dots（PeQDs） are emerging as a new generation of optoelectronic and photovoltaic materials owing to their outstanding optoelectronic properties such as long carrier diffusion distance, large absorption coefficient, high photoluminescence（PL） quantum yield（QY）, narrow emission band, and tunable band gap and PL emission by varying the halide composition. [1,2] The combination of PeQDs with rare-earth（RE） emitters may bring about new optical, electric, thermal, and magnetic properties. [3] In this talk, we shall focus on our recent efforts on the development of PeQDs and RE hybridized materials based on RE-doped PeQDs and PeQDs/RE hetero-structures. Specifically, through sensitization by RE-doped nanoparticles, we have realized full-spectrum photon upconversion tuning in all-inorganic CsPbX（X = Cl, Br, and I） PeQDs under low power density excitation, with a color gamut of 140% NTSC, upconversion QYs approaching 0.5%,and significantly lengthened exciton lifetimes from μs to ms scale. [4] We have also developed a novel strategy for fine-tuning the persistent luminescence with a color gamut of 130% NTSC and highly synchronized afterglow decay over 8 h by using CsPbX3 PeQDs as efficient afterglow light conversion materials. [5] These findings provide a general approach for tailoring the upconversion and persistent luminescence by the marriage of PeQDs with RE emitters, thereby opening up new opportunities for PeQDs and RE emitters towards many emerging applications such as solar spectrum conversion, white-emitting persistent light source,complex data storage, and multilevel anti-counterfeiting.

关键词： perovskite quantum dots rare earths energy transfer upconversion luminescence persistent luminescence

来源：评论

学校读者我要写书评

暂无评论

Dual-Band-Tunable White-Light Emission from Bi3+/Te4+Emitters in Perovskite-Derivative Cs2SnCl6Microcrystals

引用

Angewandte Chemie 2022年第9期134卷

作者： Wei Zhang Prof. Wei Zheng Dr. Lingyun Li Prof. Ping Huang Dr. Zhongliang Gong Ziwei Zhou Jinyue Sun Prof. Yan Yu Prof. Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Key Laboratory of Advanced Materials Technologies College of Materials Science and Engineering Fuzhou University Fuzhou Fujian 350108 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China

Luminescent metal halides have attracted considerable attention in next-generation solid-state lighting because of their superior optical properties and easy solution processibility. Herein, we report a new class of highly efficient and dual-band-tunable white-light emitters based on Bi 3+ /Te 4+ co-doped perovskite derivative Cs 2 SnCl 6 microcrystals. Owing to the strong electron-phonon coupling and efficient energy transfer from Bi 3+ to Te 4+ , the microcrystals exhibited broad dual-band white-light emission originating from the inter-configurational 3 P 0,1 → 1 S 0 transitions of Bi 3+ and Te 4+ , with good stability and a high photoluminescence (PL) quantum yield of up to 68.3 %. Specifically, a remarkable transition in Bi 3+ -PL lifetime from milliseconds at 10 K to microseconds at 300 K was observed, as solid evidence for the isolated Bi 3+ emission. These findings provide not only new insights into the excited-state dynamics of Bi 3+ and Te 4+ in Cs 2 SnCl 6 , but also a general approach to achieve single-composition white-light emitters based on lead-free metal halides through ns 2 -metal ion co-doping.

关键词： Bismuth Cs2SnCl6 Excited-State Dynamics Tellurium White-Light Emission

来源：评论

学校读者我要写书评

暂无评论

A Perimidin Derivative with Multiple Redox Centers as an Anode for Lithium-ion Batteries①

引用

结构化学 2020年第2期

作者： FUYu-Ru LIUQin SUNChuan-Fu CAS Key Laboratory of Design and Assembly of Functional Nanostructures，and Fujian Key Laboratory of Nanomaterials，Fujian Institute of Research on the Structure of Matter，Chinese Academy of Sciences，Fuzhou 350002，China University of Chinese Academy of Sciences，Beijing 100039，China

来源：评论

学校读者我要写书评

暂无评论

Artificial Photosynthetic Cell with Molecular Biomimetic Thylakoid

引用

Angewandte Chemie 2024年第4期137卷

作者： Enbo Zhou Shichen Yan Xiang Zhang Ateeq Ur Rehman Baloch Yangdan Hui Futong Wang Lei Jiao Jiafang Xie Prof. Daqiang Yuan Prof. Yaobing Wang Fujian Agriculture and Forestry University Fuzhou 350002 Fujian P. R. China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China Key Laboratory of Urban Pollutant Conversion Institute of Urban Environment Chinese Academy of Sciences Xiamen P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China

The construction of solar-to-chemical conversion system by mimicking the photosynthetic network of the chloroplast holds great promise on efficient solar energy utilization. We developed an artificial photosynthetic cell (APC) based on molecular biomimetic thylakoid (CoTPP-FePy) to split water into hydrogen and oxygen (H 2 and O 2 ) at low driving voltage (1.1 V) and neutral condition (pH≈7). The CoTPP-FePy can emulate the light reaction in thylakoids to produce O 2 by coupling light harvesting, photocatalysis, and electron/energy storage (Fe III /Fe II −Py). Subsequently, a membrane electrode assembly (MEA) were employed to simulate the dark reaction, wherein the proton, electron and energy generated by the light reaction can drive the H 2 producing process. By a temporally and spatially coupling of the light and dark reactions, the resulting APC achieved a solar conversion efficiency of 3.1 %, exceeding that of natural photosynthetic systems and demonstrating the potential of artificial photosynthesis.

关键词： Artificial photosynthesis Photocatalytic water oxidation Water splitting Metal organic cage Biomimetic chemistry

来源：评论

学校读者我要写书评

暂无评论

Polyoxometalate–Organic Hybrid “Calixarenes” as Supramolecular Hosts

引用

Angewandte Chemie 2023年第4期136卷

作者： Yuan Gao Dr. Ji Guo Yuyan Lai Jiaheng Lin Junrui Liu Jianming Ji Prof. Dr. Panchao Yin Prof. Dr. Wei Wang Prof. Dr. Hongmei Zhao Prof. Dr. Guanying Chen Prof. Dr. Lei Wang Prof. Dr. Xikui Fang MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 China South China Advanced Institute for Soft Matter Science and Technology State Key Laboratory of Luminescent Materials and Devices South China University of Technology Guangzhou 510640 China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China State Key Laboratory of Information Photonics and Optical Communications School of Science Beijing University of Posts and Telecommunications Beijing 100876 China

Calixarenes are among the most useful and versatile macrocycles in supramolecular chemistry. The one thing that has not changed in the 80 years since their discovery, despite numerous derivatizations, is their fully organic, covalent scaffolds. Here, we report a new type of organic–inorganic hybrid “calixarenes” constructed by means of coordination-driven assembly. Replacing acetate ligands on the {SiW 10 Cr 2 (OAc) 2 } clusters with 5-hydroxyisophthalates allows these 95° inorganic building blocks to be linked into bowl-shaped, hybrid “calix[ n ]arenes” ( n =3, 4). With a large concave cavity, the metal–organic calix[4]arene can accommodate nanometer-sized polyoxoanions in an entropically driven process. The development of hybrid variants of calixarenes is expected to expand the scope of their physicochemical properties, guest/substrate binding, and applications on multiple fronts.

关键词： Calixarenes Host–Guest Systems Macrocycles Polyoxometalates Supramolecular Chemistry

来源：评论

学校读者我要写书评

暂无评论

建议与咨询留下您的常用邮箱和电话号码，以便我们向您反馈解决方案和替代方法

时间限定

文献类型

馆藏选择

核心期刊

语言

文献类型

帮助

文字说明：

检索规则说明：

检索范例：

分类表

所选分类

限定检索结果

文献类型

馆藏范围

日期分布

学科分类号

主题

机构

作者

语言

请选择保存的检索档案：

请选择收藏分类：

通借通还

建议与咨询 留下您的常用邮箱和电话号码，以便我们向您反馈解决方案和替代方法

时间限定

文献类型

馆藏选择

核心期刊

语言

文献类型

帮助

文字说明：

检索规则说明：

检索范例：

分类表

所选分类

限定检索结果

文献类型

馆藏范围

日期分布

学科分类号

主题

机构

作者

语言

请选择保存的检索档案： 新增检索档案 确定 取消

请选择收藏分类： 新增自定义分类 确定 取消

通借通还

建议与咨询留下您的常用邮箱和电话号码，以便我们向您反馈解决方案和替代方法

请选择保存的检索档案：

请选择收藏分类：