排序方式: 共有115条查询结果,搜索用时 31 毫秒
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T. Gamze Ulusoy Ghobadi Amir Ghobadi Muhammed Buyuktemiz Elif Akhuseyin Yildiz Dilara Berna Yildiz Prof. H. Gul Yaglioglu Prof. Yavuz Dede Prof. Ekmel Ozbay Prof. Ferdi Karadas 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(10):4111-4119
Herein, we establish a simple synthetic strategy affording a heterogeneous, precious metal-free, dye-sensitized photoelectrode for water oxidation, which incorporates a Prussian blue (PB) structure for the sensitization of TiO2 and water oxidation catalysis. Our approach involves the use of a Fe(CN)5 bridging group not only as a cyanide precursor for the formation of a PB-type structure but also as an electron shuttle between an organic chromophore and the catalytic center. The resulting hetero-functional PB-modified TiO2 electrode demonstrates a low-cost and easy-to-construct photoanode, which exhibits favorable electron transfers with a remarkable excited state lifetime on the order of nanoseconds and an extended light absorption capacity of up to 500 nm. Our approach paves the way for a new family of precious metal-free robust dye-sensitized photoelectrodes for water oxidation, in which a variety of common organic chromophores can be employed in conjunction with CoFe PB structures. 相似文献
83.
Ming Shi Guanna Li Jianming Li Xu Jin Xiaoping Tao Bin Zeng Prof. Evgeny A. Pidko Prof. Rengui Li Prof. Can Li 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(16):6652-6657
Surface atomic arrangement and coordination of photocatalysts highly exposed to different crystal facets significantly affect the photoreactivity. However, controversies on the true photoreactivity of a specific facet in heterogeneous photocatalysis still exits. Herein, we exemplified well-defined BiOBr nanosheets dominating with respective facets, (001) and (010), to track the reactivity of crystal facets for photocatalytic water splitting. The real photoreactivity of BiOBr-(001) were evidenced to be significantly higher than BiOBr-(010) for both hydrogen production and oxygen evolution reactions. Further in situ photochemical probing studies verified the distinct reactivity is not only owing to the highly exposed facets, but dominated by the co-exposing facets, leading to an efficient spatial separation of photogenerated charges and further making the oxidation and reduction reactions separately occur with different reaction rates, which ordains the fate of the true photoreactivity. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(18):5143-5147
The development of cost‐effective and active water‐splitting electrocatalysts that work at mild pH is an essential step towards the realization of sustainable energy and material circulation in our society. Its success requires a drastic improvement in the kinetics of the anodic half‐reaction of the oxygen evolution reaction (OER), which determines the overall system efficiency to a large extent. A simple electrochemical protocol has been developed to activate Ni electrodes, by which a stable NiOOH phase was formed, which could weakly bind to alkali‐metal cations. The electrochemically activated (ECA) Ni electrode reached a current of 10 mA at <1.40 V vs. the reversible hydrogen electrode (RHE) at practical operation temperatures (>75 °C) and a mild pH of ca. 10 with excellent stability (>24 h), greatly surpassing that of the state‐of‐the‐art NiFeOx electrodes under analogous conditions. Water electrolysis was demonstrated with ECA‐Ni and NiMo, which required an iR‐free overall voltage of only 1.44 V to reach 10 mA cmgeo−2. 相似文献
86.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(5):1344-1348
In spite of recent advances in the synthesis of hollow micro/nanostructures, the fabrication of three‐dimensional electrodes on the basis of these structures remains a major challenge. Herein, we develop an electrochemical sacrificial‐template strategy to fabricate hollow Co3O4 microtube arrays with hierarchical porosity. The resultant unique structures and integrated electrode configurations impart enhanced mass transfer and electron mobility, ensuring high activity and stability in catalyzing oxygen and hydrogen evolution reactions. Impressively, the apparent performance can rival that of state‐of‐the‐art noble‐metal and transition‐metal electrocatalysts. Furthermore, this bifunctional electrode can be used for highly efficient overall water splitting, even competing with the integrated performance of Pt/C and IrO2/C. 相似文献
87.
Tomohiro Higashi Hiroshi Nishiyama Yohichi Suzuki Yutaka Sasaki Takashi Hisatomi Masao Katayama Tsutomu Minegishi Kazuhiko Seki Taro Yamada Kazunari Domen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(8):2322-2326
Photoelectrochemical water splitting is regarded as a promising approach to the production of hydrogen, and the development of efficient photoelectrodes is one aspect of realizing practical systems. In this work, transparent Ta3N5 photoanodes were fabricated on n‐type GaN/sapphire substrates to promote O2 evolution in tandem with a photocathode, to realize overall water splitting. Following the incorporation of an underlying GaN layer, a photocurrent of 6.3 mA cm?2 was achieved at 1.23 V vs. a reversible hydrogen electrode. The transparency of Ta3N5 to wavelengths longer than 600 nm allowed incoming solar light to be transmitted to a CuInSe2 (CIS), which absorbs up to 1100 nm. A stand‐alone tandem cell with a serially‐connected dual‐CIS unit terminated with a Pt/Ni electrode was thus constructed for H2 evolution. This tandem cell exhibited a solar‐to‐hydrogen energy conversion efficiency greater than 7 % at the initial stage of the reaction. 相似文献
88.
Dongho Choi Seong Kyung Nam Kiwon Kim Jun Hyuk Moon 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(21):6965-6969
As the performance of photoanodes for solar water splitting steadily improves, the extension of the absorption wavelength in the photoanodes is highly necessary to substantially improve the water splitting. We use a luminescent back reflector (LBR) capable of photon upconversion (UC) to improve the light harvesting capabilities of Mo:BiVO4 photoelectrodes. The LBR is prepared by dispersing the organic dye pair meso‐tetraphenyltetrabenzoporphine palladium and perylene capable of triplet–triplet annhilation‐based UC in a polymer film. The LBR converts the wavelengths of 600–650 nm corresponding to the sub‐band gap of Mo:BiVO4 and the wavelengths of 350–450 nm that are not sufficiently absorbed in Mo:BiVO4 to a wavelength that can be absorbed by a Mo:BiVO4 photoelectrode. The LBR improves the water splitting reaction of Mo:BiVO4 photoelectrodes by 17 %, and consequently, the Mo:BiVO4/LBR exhibits a photocurrent density of 5.25 mA cm?2 at 1.23 V versus the reversible hydrogen electrode. The Mo:BiVO4/LBR exhibits hydrogen/oxygen evolution corresponding to the increased photocurrent density and long‐term operational stability for the water splitting reaction. 相似文献
89.
Changhui Chen Yang Chen Ruoqing Yao Yanxi Li Chunxi Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(12):3979-3982
The natural Mn4Ca cluster in photosystem II serves as a blueprint to develop artificial water‐splitting catalysts for the generation of solar fuel in artificial photosynthesis. Although significant advances have recently been achieved, it remains a great challenge to prepare robust artificial Mn4Ca clusters that precisely mimic the structure and function of the biological catalyst. Herein, we report the isolation and structural characterization of two Mn4CaO4 complexes with polar solvent molecules, acetonitrile or N,N‐dimethylformamide, which closely mimics the two water molecules on the calcium ion, as well as the oxidation states of the four manganese ions and the main geometric structure of the natural Mn4Ca cluster. These new artificial Mn4Ca complexes provide important chemical clues to understand the structure and mechanism of the biological system. 相似文献
90.
Jintao Zhang Liming Dai 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2016,128(42):13490-13494
Electrocatalysts are required for clean energy technologies (for example, water‐splitting and metal‐air batteries). The development of a multifunctional electrocatalyst composed of nitrogen, phosphorus, and fluorine tri‐doped graphene is reported, which was obtained by thermal activation of a mixture of polyaniline‐coated graphene oxide and ammonium hexafluorophosphate (AHF). It was found that thermal decomposition of AHF provides nitrogen, phosphorus, and fluorine sources for tri‐doping with N, P, and F, and simultaneously facilitates template‐free formation of porous structures as a result of thermal gas evolution. The resultant N, P, and F tri‐doped graphene exhibited excellent electrocatalytic activities for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The trifunctional metal‐free catalyst was further used as an OER–HER bifunctional catalyst for oxygen and hydrogen gas production in an electrochemical water‐splitting unit, which was powered by an integrated Zn–air battery based on an air electrode made from the same electrocatalyst for ORR. The integrated unit, fabricated from the newly developed N, P, and F tri‐doped graphene multifunctional metal‐free catalyst, can operate in ambient air with a high gas production rate of 0.496 and 0.254 μL s−1 for hydrogen and oxygen gas, respectively, showing great potential for practical applications. 相似文献