共查询到20条相似文献,搜索用时 15 毫秒
1.
Dr. Kosuke Suzuki Fei Tang Dr. Yuji Kikukawa Dr. Kazuya Yamaguchi Prof. Dr. Noritaka Mizuno 《Angewandte Chemie (International ed. in English)》2014,53(21):5356-5360
The development of visible‐light‐induced photocatalysts for chemoselective functional group transformations has received considerable attention. Polyoxometalates (POMs) are potential materials for efficient photocatalysts because their properties can be precisely tuned by changing their constituent elements and structures and by the introduction of additional metal cations. Furthermore, they are thermally and oxidatively more stable than the frequently utilized organometallic complexes. The visible‐light‐responsive tetranuclear cerium(III)‐containing silicotungstate TBA6[{Ce(H2O)}2{Ce(CH3CN)}2(μ4‐O)(γ‐SiW10O36)2] (CePOM; TBA=tetra‐n‐butylammonium) has now been synthesized; when CePOM was irradiated with visible light (λ>400 nm), a unique intramolecular CeIII‐to‐POM(WVI) charge transfer was observed. With CePOM, the photocatalytic oxidative dehydrogenation of primary and secondary amines as well as the α‐cyanation of tertiary amines smoothly proceeded in the presence of O2 (1 atm) as the sole oxidant. 相似文献
2.
Efficient Visible‐Light‐Driven CO2 Reduction Mediated by Defect‐Engineered BiOBr Atomic Layers
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Ju Wu Xiaodong Li Wen Shi Peiquan Ling Prof. Yongfu Sun Xingchen Jiao Dr. Shan Gao Liang Liang Jiaqi Xu Prof. Wensheng Yan Dr. Chengming Wang Prof. Yi Xie 《Angewandte Chemie (International ed. in English)》2018,57(28):8719-8723
Solar CO2 reduction efficiency is largely limited by poor photoabsorption, sluggish electron–hole separation, and a high CO2 activation barrier. Defect engineering was employed to optimize these crucial processes. As a prototype, BiOBr atomic layers were fabricated and abundant oxygen vacancies were deliberately created on their surfaces. X‐ray absorption near‐edge structure and electron paramagnetic resonance spectra confirm the formation of oxygen vacancies. Theoretical calculations reveal the creation of new defect levels resulting from the oxygen vacancies, which extends the photoresponse into the visible‐light region. The charge delocalization around the oxygen vacancies contributes to CO2 conversion into COOH* intermediate, which was confirmed by in situ Fourier‐transform infrared spectroscopy. Surface photovoltage spectra and time‐resolved fluorescence emission decay spectra indicate that the introduced oxygen vacancies promote the separation of carriers. As a result, the oxygen‐deficient BiOBr atomic layers achieve visible‐light‐driven CO2 reduction with a CO formation rate of 87.4 μmol g?1 h?1, which was not only 20 and 24 times higher than that of BiOBr atomic layers and bulk BiOBr, respectively, but also outperformed most previously reported single photocatalysts under comparable conditions. 相似文献
3.
Hongjian Yu Jieyuan Li Yihe Zhang Songqiu Yang Keli Han Fan Dong Tianyi Ma Hongwei Huang 《Angewandte Chemie (International ed. in English)》2019,58(12):3880-3884
A facile and controllable in situ reduction strategy is used to create surface oxygen vacancies (OVs) on Aurivillius‐phase Sr2Bi2Nb2TiO12 nanosheets, which were prepared by a mineralizer‐assisted soft‐chemical method. Introduction of OVs on the surface of Sr2Bi2Nb2TiO12 extends photoresponse to cover the whole visible region and also tremendously promotes separation of photoinduced charge carriers. Adsorption and activation of CO2 molecules on the surface of the catalyst are greatly enhanced. In the gas‐solid reaction system without co‐catalysts or sacrificial agents, OVs‐abundant Sr2Bi2Nb2TiO12 nanosheets show outstanding CO2 photoreduction activity, producing CO with a rate of 17.11 μmol g?1 h?1, about 58 times higher than that of the bulk counterpart, surpassing most previously reported state‐of‐the‐art photocatalysts. Our study provides a three‐in‐one integrated solution to advance the performance of photocatalysts for solar‐energy conversion and generation of renewable energy. 相似文献
4.
Kai Zhang Liang‐Qiu Lu Yue Jia Ying Wang Fu‐Dong Lu Fangfang Pan Wen‐Jing Xiao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(38):13509-13513
Chiral catalysts tolerating photochemical reactions are in great demand for the vast development of visible‐light‐induced asymmetric synthesis. Now, chiral octahedral complexes based on earth‐abundant metal and chiral N4 ligands are reported. One well‐defined chiral CoII‐complex is shown to be an efficient catalyst in the visible‐light‐induced conjugated addition of enones by alkyl and acyl radicals, providing synthetically valued chiral ketones and 1,4‐dicarbonyls in 47–>99 % yields with up to 97:3 e.r. 相似文献
5.
Hongjian Yu Jieyuan Li Yihe Zhang Songqiu Yang Keli Han Fan Dong Tianyi Ma Hongwei Huang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(12):3920-3924
A facile and controllable in situ reduction strategy is used to create surface oxygen vacancies (OVs) on Aurivillius‐phase Sr2Bi2Nb2TiO12 nanosheets, which were prepared by a mineralizer‐assisted soft‐chemical method. Introduction of OVs on the surface of Sr2Bi2Nb2TiO12 extends photoresponse to cover the whole visible region and also tremendously promotes separation of photoinduced charge carriers. Adsorption and activation of CO2 molecules on the surface of the catalyst are greatly enhanced. In the gas‐solid reaction system without co‐catalysts or sacrificial agents, OVs‐abundant Sr2Bi2Nb2TiO12 nanosheets show outstanding CO2 photoreduction activity, producing CO with a rate of 17.11 μmol g?1 h?1, about 58 times higher than that of the bulk counterpart, surpassing most previously reported state‐of‐the‐art photocatalysts. Our study provides a three‐in‐one integrated solution to advance the performance of photocatalysts for solar‐energy conversion and generation of renewable energy. 相似文献
6.
Yan Wang Sibo Wang Song Lin Zhang Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2020,59(29):11918-11922
Hierarchical FeCoS2–CoS2 double‐shelled nanotubes have been rationally designed and constructed for efficient photocatalytic CO2 reduction under visible light. The synthetic strategy, engaging the two‐step cation‐exchange reactions, precisely integrates two metal sulfides into a double‐shelled tubular heterostructure with both of the shells assembled from ultrathin two‐dimensional (2D) nanosheets. Benefiting from the distinctive structure and composition, the FeCoS2–CoS2 hybrid can reduce bulk‐to‐surface diffusion length of photoexcited charge carriers to facilitate their separation. Furthermore, this hybrid structure can expose abundant active sites for enhancing CO2 adsorption and surface‐dependent redox reactions, and harvest incident solar irradiation more efficiently by light scattering in the complex interior. As a result, these hierarchical FeCoS2–CoS2 double‐shelled nanotubes exhibit superior activity and high stability for photosensitized deoxygenative CO2 reduction, affording a high CO‐generating rate of 28.1 μmol h?1 (per 0.5 mg of catalyst). 相似文献
7.
Constructing Ordered Three‐Dimensional TiO2 Channels for Enhanced Visible‐Light Photocatalytic Performance in CO2 Conversion Induced by Au Nanoparticles
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Dr. Hairong Xue Prof. Dr. Tao Wang Hao Gong Hu Guo Xiaoli Fan Bin Gao Yaya Feng Prof. Dr. Xianguang Meng Prof. Dr. Xianli Huang Prof. Dr. Jianping He 《化学:亚洲杂志》2018,13(5):577-583
As a typical photocatalyst for CO2 reduction, practical applications of TiO2 still suffer from low photocatalytic efficiency and limited visible‐light absorption. Herein, a novel Au‐nanoparticle (NP)‐decorated ordered mesoporous TiO2 (OMT) composite (OMT‐Au) was successfully fabricated, in which Au NPs were uniformly dispersed on the OMT. Due to the surface plasmon resonance (SPR) effect derived from the excited Au NPs, the TiO2 shows high photocatalytic performance for CO2 reduction under visible light. The ordered mesoporous TiO2 exhibits superior material and structure, with a high surface area that offers more catalytically active sites. More importantly, the three‐dimensional transport channels ensure the smooth flow of gas molecules, highly efficient CO2 adsorption, and the fast and steady transmission of hot electrons excited from the Au NPs, which lead to a further improvement in the photocatalytic performance. These results highlight the possibility of improving the photocatalysis for CO2 reduction under visible light by constructing OMT‐based Au‐SPR‐induced photocatalysts. 相似文献
8.
Dr. Yoshinobu Kamakura Dr. Chomponoot Suppaso Issei Yamamoto Ryusuke Mizuochi Yusuke Asai Prof. Dr. Teruki Motohashi Prof. Dr. Daisuke Tanaka Prof. Dr. Kazuhiko Maeda 《Angewandte Chemie (International ed. in English)》2023,62(28):e202305923
Certain metal complexes are known as high-performance CO2 reduction photocatalysts driven by visible light. However, most of them rely on rare, precious metals as principal components, and integrating the functions of light absorption and catalysis into a single molecular unit based on abundant metals remains a challenge. Metal-organic frameworks (MOFs), which can be regarded as intermediate compounds between molecules and inorganic solids, are potential platforms for the construction of a simple photocatalytic system composed only of Earth-abundant nontoxic elements. In this work, we report that a tin-based MOF enables the conversion of CO2 into formic acid with a record high apparent quantum yield (9.8 % at 400 nm) and >99 % selectivity without the need for any additional photosensitizer or catalyst. This work highlights a new MOF with strong potential for photocatalytic CO2 reduction driven by solar energy. 相似文献
9.
One‐pot Synthesis of CdS Nanocrystals Hybridized with Single‐Layer Transition‐Metal Dichalcogenide Nanosheets for Efficient Photocatalytic Hydrogen Evolution
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Junze Chen Dr. Xue‐Jun Wu Lisha Yin Dr. Bing Li Dr. Xun Hong Zhanxi Fan Bo Chen Prof. Can Xue Prof. Hua Zhang 《Angewandte Chemie (International ed. in English)》2015,54(4):1210-1214
Exploration of low‐cost and earth‐abundant photocatalysts for highly efficient solar photocatalytic water splitting is of great importance. Although transition‐metal dichalcogenides (TMDs) showed outstanding performance as co‐catalysts for the hydrogen evolution reaction (HER), designing TMD‐hybridized photocatalysts with abundant active sites for the HER still remains challenge. Here, a facile one‐pot wet‐chemical method is developed to prepare MS2–CdS (M=W or Mo) nanohybrids. Surprisedly, in the obtained nanohybrids, single‐layer MS2 nanosheets with lateral size of 4–10 nm selectively grow on the Cd‐rich (0001) surface of wurtzite CdS nanocrystals. These MS2–CdS nanohybrids possess a large number of edge sites in the MS2 layers, which are active sites for the HER. The photocatalytic performances of WS2–CdS and MoS2–CdS nanohybrids towards the HER under visible light irradiation (>420 nm) are about 16 and 12 times that of pure CdS, respectively. Importantly, the MS2–CdS nanohybrids showed enhanced stability after a long‐time test (16 h), and 70 % of catalytic activity still remained. 相似文献
10.
Dengrong Sun Dr. Yanghe Fu Wenjun Liu Lin Ye Dengke Wang Lin Yang Prof. Dr. Xianzhi Fu Prof. Dr. Zhaohui Li 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(42):14279-14285
Metal–organic framework (MOF) NH2‐Uio‐66(Zr) exhibits photocatalytic activity for CO2 reduction in the presence of triethanolamine as sacrificial agent under visible‐light irradiation. Photoinduced electron transfer from the excited 2‐aminoterephthalate (ATA) to Zr oxo clusters in NH2‐Uio‐66(Zr) was for the first time revealed by photoluminescence studies. Generation of ZrIII and its involvement in photocatalytic CO2 reduction was confirmed by ESR analysis. Moreover, NH2‐Uio‐66(Zr) with mixed ATA and 2,5‐diaminoterephthalate (DTA) ligands was prepared and shown to exhibit higher performance for photocatalytic CO2 reduction due to its enhanced light adsorption and increased adsorption of CO2. This study provides a better understanding of photocatalytic CO2 reduction over MOF‐based photocatalysts and also demonstrates the great potential of using MOFs as highly stable, molecularly tunable, and recyclable photocatalysts in CO2 reduction. 相似文献
11.
Michael Neumeier Uttam Chakraborty Dieter Schaarschmidt Victor de la Pena O'Shea Raul Perez‐Ruiz Axel Jacobi von Wangelin 《Angewandte Chemie (International ed. in English)》2020,59(32):13473-13478
Successful combinations of visible‐light photocatalysis with metal catalysis have recently enabled the development of hitherto unknown chemical reactions. Dual mechanisms from merging metal‐free photocatalysts and earth‐abundant metal catalysts are still in their infancy. We report a photo‐organo‐iron‐catalyzed cyclotrimerization of alkynes by photoredox activation of a ligand‐free Fe catalyst. The reaction operates under very mild conditions (visible light, 20 °C, 1 h) with 1–2 mol % loading of the three catalysts (dye, amine, FeCl2). 相似文献
12.
CO2‐Triggered Switchable Hydrophilicity of a Heterogeneous Conjugated Polymer Photocatalyst for Enhanced Catalytic Activity in Water
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Dr. Jeehye Byun Wei Huang Di Wang Run Li Dr. Kai A. I. Zhang 《Angewandte Chemie (International ed. in English)》2018,57(11):2967-2971
Water compatibility for heterogeneous photocatalysts has been pursued for energy and environmental applications. However, there exists a trade‐off between hydrophilicity and recyclability of the photocatalyst. Herein, we report a conjugated polymer photocatalyst with tertiary amine terminals that reversibly binds CO2 in water, thereby generating switchable hydrophilicity. The CO2‐assisted hydrophilicity boosted the photocatalytic efficiency in aqueous medium with minimum dosage. When CO2 was desorbed, the photocatalyst could be simply regenerated from reaction media, facilitating the repeated use of photocatalyst. Hydrophilicity/hydrophobicity control of the polymer photocatalyst was successfully showcased through a variety of organic photoredox reactions under visible‐light irradiation in water. 相似文献
13.
Highly Dispersed Polyoxometalate‐Doped Porous Co3O4 Water Oxidation Photocatalysts Derived from POM@MOF Crystalline Materials
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Qing Lan Dr. Zhi‐Ming Zhang Dr. Chao Qin Prof. Xin‐Long Wang Prof. Yang‐Guang Li Dr. Hua‐Qiao Tan Prof. En‐Bo Wang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(43):15513-15520
Rational design of earth‐abundant photocatalysts is an important issue for solar energy conversion and storage. Polyoxometalate (POM)@Co3O4 composites doped with highly dispersive molecular metal–oxo clusters, synthesized by loading a single Keggin‐type POM cluster into each confined space of a metal–organic framework (MOF), exhibit significantly improved photocatalytic activity in water oxidation compared to the pure MOF‐derived nanostructure. The systematic synthesis of these composite nanocrystals allows the conditions to be tuned, and their respective water oxidation catalytic performance can be efficiently adjusted by varying the thermal treatment temperature and the feeding amount of the POM. This work not only provides a modular and tunable synthetic strategy for preparing molecular cluster@TM oxide (TM=transition metal) nanostructures, but also showcases a universal strategy that is applicable to design and construct multifunctional nanoporous metal oxide composite materials. 相似文献
14.
Xiaoxiao Yu Zhenzhen Yang Bing Qiu Shien Guo Peng Yang Bo Yu Hongye Zhang Yanfei Zhao Xinzheng Yang Buxing Han Zhimin Liu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(2):642-646
Visible‐light‐driven photoreduction of CO2 to energy‐rich chemicals in the presence of H2O without any sacrifice reagent is of significance, but challenging. Herein, Eosin Y‐functionalized porous polymers (PEosinY‐N, N=1–3), with high surface areas up to 610 m2 g?1, are reported. They exhibit high activity for the photocatalytic reduction of CO2 to CO in the presence of gaseous H2O, without any photosensitizer or sacrifice reagent, and under visible‐light irradiation. Especially, PEosinY‐1 derived from coupling of Eosin Y with 1,4‐diethynylbenzene shows the best performance for the CO2 photoreduction, affording CO as the sole carbonaceous product with a production rate of 33 μmol g?1 h?1 and a selectivity of 92 %. This work provides new insight for designing and fabricating photocatalytically active polymers with high efficiency for solar‐energy conversion. 相似文献
15.
Visible‐Light‐Driven CO2 Reduction with Carbon Nitride: Enhancing the Activity of Ruthenium Catalysts
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Ryo Kuriki Dr. Keita Sekizawa Prof. Dr. Osamu Ishitani Prof. Dr. Kazuhiko Maeda 《Angewandte Chemie (International ed. in English)》2015,54(8):2406-2409
A heterogeneous photocatalyst system that consists of a ruthenium complex and carbon nitride (C3N4), which act as the catalytic and light‐harvesting units, respectively, was developed for the reduction of CO2 into formic acid. Promoting the injection of electrons from C3N4 into the ruthenium unit as well as strengthening the electronic interactions between the two units enhanced its activity. The use of a suitable solvent further improved the performance, resulting in a turnover number of greater than 1000 and an apparent quantum yield of 5.7 % at 400 nm. These are the best values that have been reported for heterogeneous photocatalysts for CO2 reduction under visible‐light irradiation to date. 相似文献
16.
Kai‐Kai Chen Song Guo Heyuan Liu Xiyou Li Zhi‐Ming Zhang Tong‐Bu Lu 《Angewandte Chemie (International ed. in English)》2020,59(31):12951-12957
Developing strong visible‐light‐absorbing (SVLA) earth‐abundant photosensitizers (PSs) for significantly improving the utilization of solar energy is highly desirable, yet it remains a great challenge. Herein, we adopt a through‐bond energy transfer (TBET) strategy by bridging boron dipyrromethene (Bodipy) and a CuI complex with an electronically conjugated bridge, resulting in the first SVLA CuI PSs ( Cu‐2 and Cu‐3 ). Cu‐3 has an extremely high molar extinction coefficient of 162 260 m ?1 cm?1 at 518 nm, over 62 times higher than that of traditional CuI PS ( Cu‐1 ). The photooxidation activity of Cu‐3 is much greater than that of Cu‐1 and noble‐metal PSs (Ru(bpy)32+ and Ir(ppy)3+) for both energy‐ and electron‐transfer reactions. Femto‐ and nanosecond transient absorption and theoretical investigations demonstrate that a “ping‐pong” energy‐transfer process in Cu‐3 involving a forward singlet TBET from Bodipy to the CuI complex and a backward triplet‐triplet energy transfer greatly contribute to the long‐lived and Bodipy‐localized triplet excited state. 相似文献
17.
Tailoring the Optical Absorption of Water‐Stable ZrIV‐ and HfIV‐Based Metal–Organic Framework Photocatalysts
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Tan L. H. Doan Ha L. Nguyen Hung Q. Pham Nguyen‐Nguyen Pham‐Tran Prof. Thach N. Le Kyle E. Cordova 《化学:亚洲杂志》2015,10(12):2660-2668
New ZrIV‐ and HfIV‐based metal–organic framework photocatalysts, termed VNU‐1 and VNU‐2 (where VNU=Vietnam National University), were synthesized and their resulting structures fully characterized. By employing a highly π‐conjugated linker, namely 1,4‐bis(2‐[4‐carboxyphenyl]ethynyl)benzene, the optical absorption properties were effectively red‐shifted into the visible light region. This strategy, coupled with the high water stability of the materials, led to enhanced MOF‐driven photocatalytic degradation, under ultraviolet‐visible light, of organic dye pollutants commonly found in wastewater. 相似文献
18.
Metal Complexes Supported on Solid Matrices for Visible‐Light‐Driven Molecular Transformations
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Prof. Dr. Kohsuke Mori Prof. Dr. Hiromi Yamashita 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(32):11122-11137
Hybridization of visible‐light‐responsive metal complexes with solid matrices offers an attractive route for practical catalyst design of nanostructured photocatalysts that are operationally simple and can attain unprecedented reactions owing to synergistic effects. This Minireview highlights the precise architectures of hybrid photocatalysts that enable efficient and selective photochemical molecular transformations, including selective oxidation by O2 and H2 evolution from water. Several techniques for the immobilization of metal complexes are discussed, including encapsulation within zeolite cavities, anchoring within mesoporous channels, incorporation within the macroreticular space of ion‐exchange resins, intercalation within the interlayer spaces of layered materials, and anchoring onto the plasmonic colloidal Ag nanoparticles. The relationships between photoluminescence characteristics and photocatalytic activities of these hybrid materials are also discussed. 相似文献
19.
Nauman Ali Amir Zada Muhammad Zahid Ahmed Ismail Misbha Rafiq Aaisha Riaz Adnan Khan 《中国化学会会志》2019,66(4):402-408
It is highly desired to synthesize low‐cost photocatalysts for the degradation of colored dyes to safeguard our environment for the future generations. Here, we report an extremely efficient and low‐cost synthesis of alkaline earth and transition‐metal ferrite photocatalysts (MgFe2O4, CaFe2O4, BaFe12O19, CuFe2O4, and ZnFe2O4) from their chloride salts and their applications for the degradation of methylene blue (MB) dye under UV–visible and direct sunlight irradiation. The as‐prepared photocatalysts displayed enhanced photoactivities under both conditions of irradiation. After calcination at 600°C, the photocatalytic degradation increased significantly, and 96 and 85% MB was removed with ZnFe2O4 under UV–visible and direct sunlight irradiation, respectively. Moreover, large amounts of hydroxyl free radicals were produced under both irradiation conditions, which participated in the degradation of MB. The enhanced photodegradation activities of these photocatalysts are attributed to their extended visible light absorption and low bandgaps. This work will provide a feasible route to the synthesis of efficient and low‐cost photocatalysts to utilize sunlight for environmental remediation. 相似文献
20.
Structural Design Principle of Small‐Molecule Organic Semiconductors for Metal‐Free,Visible‐Light‐Promoted Photocatalysis
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Lei Wang Wei Huang Run Li Dr. Dominik Gehrig Prof. Paul W. M. Blom Prof. Katharina Landfester Dr. Kai A. I. Zhang 《Angewandte Chemie (International ed. in English)》2016,55(33):9783-9787
Herein, we report on the structural design principle of small‐molecule organic semiconductors as metal‐free, pure organic and visible light‐active photocatalysts. Two series of electron‐donor and acceptor‐type organic semiconductor molecules were synthesized to meet crucial requirements, such as 1) absorption range in the visible region, 2) sufficient photoredox potential, and 3) long lifetime of photogenerated excitons. The photocatalytic activity was demonstrated in the intermolecular C?H functionalization of electron‐rich heteroaromates with malonate derivatives. A mechanistic study of the light‐induced electron transport between the organic photocatalyst, substrate, and the sacrificial agent are described. With their tunable absorption range and defined energy‐band structure, the small‐molecule organic semiconductors could offer a new class of metal‐free and visible light‐active photocatalysts for chemical reactions. 相似文献