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1.
Overall Water Splitting on the Transition‐Metal Oxynitride Photocatalyst LaMg1/3Ta2/3O2N over a Large Portion of the Visible‐Light Spectrum
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Dr. Chengsi Pan Dr. Tsuyoshi Takata Prof. Kazunari Domen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(5):1854-1862
One of the main targets of studies on water splitting photocatalysts is to develop semiconductor materials with narrower bandgaps capable of overall water splitting for efficient harvesting of solar energy. A series of transition‐metal oxynitrides, LaMgxTa1?xO1+3xN2?3x (x≥1/3), with a complex perovskite structure was reported as the first example of overall water splitting operable at up to 600 nm. The photocatalytic behavior of LaMg1/3Ta2/3O2N was investigated in detail in order to optimize photocatalyst preparation and water‐splitting activity. Various attempts exploring photocatalyst preparation steps, that is, cocatalyst selection, coating material and method, and synthesis method for the oxide precursor, revealed photocatalyst structures necessary for achieving overall water splitting. Careful examination of photocatalyst preparation procedures likely enhanced the quality of the produced photocatalyst, leading to a more homogeneous coating quality and semiconductor particles with fewer defects. Thus, the photocatalytic activity for water splitting on LaMg1/3Ta2/3O2N was largely enhanced. 相似文献
2.
Efficient Visible‐Light‐Driven Z‐Scheme Overall Water Splitting Using a MgTa2O6−xNy /TaON Heterostructure Photocatalyst for H2 Evolution
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Shanshan Chen Yu Qi Dr. Takashi Hisatomi Qian Ding Tomohiro Asai Zheng Li Dr. Su Su Khine Ma Prof. Fuxiang Zhang Prof. Kazunari Domen Prof. Can Li 《Angewandte Chemie (International ed. in English)》2015,54(29):8498-8501
An (oxy)nitride‐based heterostructure for powdered Z‐scheme overall water splitting is presented. Compared with the single MgTa2O6?xNy or TaON photocatalyst, a MgTa2O6?xNy /TaON heterostructure fabricated by a simple one‐pot nitridation route was demonstrated to effectively suppress the recombination of carriers by efficient spatial charge separation and decreased defect density. By employing Pt‐loaded MgTa2O6?xNy /TaON as a H2‐evolving photocatalyst, a Z‐scheme overall water splitting system with an apparent quantum efficiency (AQE) of 6.8 % at 420 nm was constructed (PtOx‐WO3 and IO3?/I? pairs were used as an O2‐evolving photocatalyst and a redox mediator, respectively), the activity of which is circa 7 or 360 times of that using Pt‐TaON or Pt‐MgTa2O6?xNy as a H2‐evolving photocatalyst, respectively. To the best of our knowledge, this is the highest AQE among the powdered Z‐scheme overall water splitting systems ever reported. 相似文献
3.
Su Su Khine Ma Prof. Kazuhiko Maeda Dr. Takashi Hisatomi Masashi Tabata Prof. Akihiko Kudo Prof. Kazunari Domen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(23):7480-7486
Tantalum nitride (Ta3N5) modified with various O2‐evolution cocatalysts was employed as a photocatalyst for water oxidation under visible light (λ>420 nm) in an attempt to construct a redox‐mediator‐free Z‐scheme water‐splitting system. Ta3N5 was prepared by nitriding Ta2O5 powder under a flow of NH3 at 1023–1223 K. The activity of Ta3N5 for water oxidation from an aqueous AgNO3 solution as an electron acceptor without cocatalyst was dependent on the generation of a well‐crystallized Ta3N5 phase with a low density of anionic defects. Modification of Ta3N5 with nanoparticulate metal oxides as cocatalysts for O2 evolution improved water‐oxidation activity. Of the cocatalysts examined, cobalt oxide (CoOx) was found to be the most effective, improving the water‐oxidation efficiency of Ta3N5 by six to seven times. Further modification of CoOx/Ta3N5 with metallic Ir as an electron sink allowed one to achieve Z‐scheme water splitting under simulated sunlight through interparticle electron transfer without the need for a shuttle redox mediator in combination with Ru‐loaded SrTiO3 doped with Rh as a H2‐evolution photocatalyst. 相似文献
4.
Wataru Kurashige Yutaro Mori Shuhei Ozaki Masanobu Kawachi Sakiat Hossain Tokuhisa Kawawaki Cameron J. Shearer Akihide Iwase Gregory F. Metha Seiji Yamazoe Akihiko Kudo Yuichi Negishi 《Angewandte Chemie (International ed. in English)》2020,59(18):7076-7082
The activity of many water‐splitting photocatalysts could be improved by the use of RhIII–CrIII mixed oxide (Rh2?xCrxO3) particles as cocatalysts. Although further improvement of water‐splitting activity could be achieved if the size of the Rh2?xCrxO3 particles was decreased further, it is difficult to load ultrafine (<2 nm) Rh2?xCrxO3 particles onto a photocatalyst by using conventional loading methods. In this study, a new loading method was successfully established and was used to load Rh2?xCrxO3 particles with a size of approximately 1.3 nm and a narrow size distribution onto a BaLa4Ti4O15 photocatalyst. The obtained photocatalyst exhibited an apparent quantum yield of 16 %, which is the highest achieved for BaLa4Ti4O15 to date. Thus, the developed loading technique of Rh2?xCrxO3 particles is extremely effective at improving the activity of the water‐splitting photocatalyst BaLa4Ti4O15. This method is expected to be extended to other advanced water‐splitting photocatalysts to achieve higher quantum yields. 相似文献
5.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(17):4817-4821
Ta3N5 is a very promising photocatalyst for solar water splitting because of its wide spectrum solar energy utilization up to 600 nm and suitable energy band position straddling the water splitting redox reactions. However, its development has long been impeded by poor compatibility with electrolytes. Herein, we demonstrate a simple sputtering‐nitridation process to fabricate high‐performance Ta3N5 film photoanodes owing to successful synthesis of the vital TaOδ precursors. An effective GaN coating strategy is developed to remarkably stabilize Ta3N5 by forming a crystalline nitride‐on‐nitride structure with an improved nitride/electrolyte interface. A stable, high photocurrent density of 8 mA cm−2 was obtained with a CoPi/GaN/Ta3N5 photoanode at 1.2 VRHE under simulated sunlight, with O2 and H2 generated at a Faraday efficiency of unity over 12 h. Our vapor‐phase deposition method can be used to fabricate high‐performance (oxy)nitrides for practical photoelectrochemical applications. 相似文献
6.
Min Wang Jia‐Qi Wang Cong Xi Chuan‐Qi Cheng Cheng‐Qin Zou Rui Zhang Ya‐Meng Xie Zhong‐Lu Guo Cheng‐Chun Tang Cun‐Ku Dong Yong‐Jun Chen Xi‐Wen Du 《Angewandte Chemie (International ed. in English)》2020,59(28):11510-11515
Developing highly efficient and low‐cost photocatalysts for overall water splitting has long been a pursuit for converting solar power into clean hydrogen energy. Herein, we demonstrate that a nonstoichiometric nickel–cobalt double hydroxide can achieve overall water splitting by itself upon solar light irradiation, avoiding the consumption of noble‐metal co‐catalysts. We employed an intensive laser to ablate a NiCo alloy target immersed in alkaline solution, and produced so‐called L‐NiCo nanosheets with a nonstoichiometric composition and O2?/Co3+ ions exposed on the surface. The nonstoichiometric composition broadens the band gap, while O2? and Co3+ ions boost hydrogen and oxygen evolution, respectively. As such, the photocatalyst achieves a H2 evolution rate of 1.7 μmol h?1 under AM 1.5G sunlight irradiation and an apparent quantum yield (AQE) of 1.38 % at 380 nm. 相似文献
7.
Perovskite Oxide Nanosheets with Tunable Band‐Edge Potentials and High Photocatalytic Hydrogen‐Evolution Activity
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Prof. Dr. Kazuhiko Maeda Dr. Miharu Eguchi Takayoshi Oshima 《Angewandte Chemie (International ed. in English)》2014,53(48):13164-13168
Perovskite nanosheets of HCa2?xSrxNb3O10 and HCa2Nb3?yTayO10 with controlled band‐edge potentials were prepared. They worked as highly efficient heterogeneous photocatalysts for H2 evolution from a water/methanol mixture under band‐gap irradiation. The activity was found to depend on the composition. The highest activity was obtained with HCa2Nb2TaO10 nanosheets, recording an apparent quantum yield of approximately 80 % at 300 nm, which is the highest value for a nanosheet‐based photocatalyst reported to date. 相似文献
8.
Interface Engineering of a CoOx/Ta3N5 Photocatalyst for Unprecedented Water Oxidation Performance under Visible‐Light‐Irradiation
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Shanshan Chen Dr. Shuai Shen Guiji Liu Yu Qi Prof. Fuxiang Zhang Prof. Can Li 《Angewandte Chemie (International ed. in English)》2015,54(10):3047-3051
Cocatalysts have been extensively used to promote water oxidation efficiency in solar‐to‐chemical energy conversion, but the influence of interface compatibility between semiconductor and cocatalyst has been rarely addressed. Here we demonstrate a feasible strategy of interface wettability modification to enhance water oxidation efficiency of the state‐of‐the‐art CoOx/Ta3N5 system. When the hydrophobic feature of a Ta3N5 semiconductor was modulated to a hydrophilic one by in situ or ex situ surface coating with a magnesia nanolayer (2–5 nm), the interfacial contact between the hydrophilic CoOx cocatalyst and the modified hydrophilic Ta3N5 semiconductor was greatly improved. Consequently, the visible‐light‐driven photocatalytic oxygen evolution rate of the resulting CoOx/MgO(in)–Ta3N5 photocatalyst is ca. 23 times that of the pristine Ta3N5 sample, with a new record (11.3 %) of apparent quantum efficiency (AQE) under 500–600 nm illumination. 相似文献
9.
Enhanced Photocatalytic Hydrogen‐Production Performance of Graphene–ZnxCd1−xS Composites by Using an Organic S Source
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Dr. Qin Li Huan Meng Prof. Jiaguo Yu Prof. Wei Xiao Yingqiu Zheng Juan Wang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(4):1176-1185
In response to the increasing concerns over energy and environmental sustainability, photocatalytic water‐splitting technology has attracted broad attention for its application in directly converting solar energy to valuable hydrogen (H2) energy. In this study, high‐efficiency visible‐light‐driven photocatalytic H2 production without the assistance of precious‐metal cocatalysts was achieved on graphene–ZnxCd1?xS composites with controlled compositions. The graphene‐ZnxCd1?xS composites were for the first time fabricated by a one‐step hydrothermal method with thiourea as an organic S source. It was found that thiourea facilitates heterogeneous nucleation of ZnxCd1?xS and in situ growth of ZnxCd1?xS nanoparticles on graphene nanosheets. Such a scenario results in abundant and intimate interfacial contact between graphene and ZnxCd1?xS nanoparticles, efficient transfer of the photogenerated charge carriers, and enhanced photocatalytic activity for H2 production. The highest H2‐production rate of 1.06 mmol h?1 g?1 was achieved on a graphene–Zn0.5Cd0.5S composite photocatalyst with a graphene content of 0.5 wt %, and the apparent quantum efficiency was 19.8 % at 420 nm. In comparison, the graphene–ZnxCd1?xS composite photocatalyst prepared by using an inorganic S source such as Na2S exhibited much lower activity for photocatalytic H2 production. In this case, homogeneous nucleation of ZnxCd1?xS becomes predominant and results in insufficient and loose contact with the graphene backbone through weak van der Waals forces and a large particle size. This study highlights the significance of the choice of S source in the design and fabrication of advanced graphene‐based sulfide photocatalytic materials with enhanced activity for photocatalytic H2 production. 相似文献
10.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(32):9440-9445
An active and stable photocatalyst to directly split water is desirable for solar‐energy conversion. However, it is difficult to accomplish overall water splitting without sacrificial electron donors. Herein, we demonstrate a strategy via constructing a single site to simultaneously promote charge separation and catalytic activity for robust overall water splitting. A single Co1‐P4 site confined on g‐C3N4 nanosheets was prepared by a facile phosphidation method, and identified by electron microscopy and X‐ray absorption spectroscopy. This coordinatively unsaturated Co site can effectively suppress charge recombination and prolong carrier lifetime by about 20 times relative to pristine g‐C3N4, and boost water molecular adsorption and activation for oxygen evolution. This single‐site photocatalyst exhibits steady and high water splitting activity with H2 evolution rate up to 410.3 μmol h−1 g−1, and quantum efficiency as high as 2.2 % at 500 nm. 相似文献
11.
The development of cocatalysts promoting overall water splitting on (Ga1−x
Zn
x
)(N1−x
O
x
) solid solution photocatalyst is presented. The (Ga1−x
Zn
x
)(N1−x
O
x
) is a stable visible-light-driven photocatalyst for stoichiometric water splitting upon loading with a suitable nanoparticulate
cocatalyst. Loading with a combination of Cr and Rh oxides, Rh2−y
Cr
y
O3, is demonstrated to raise the quantum efficiency of (Ga1−x
Zn
x
)(N1−x
O
x
) for overall water splitting to 2.5% at 420–440 nm. This represents a 10-fold increase in efficiency over the highest efficiency
previously obtained using nanoparticulate RuO2 as a cocatalyst. In addition to the composition, the dispersion and size of cocatalyst nanoparticles are identified as important
factors affecting the degree of enhancement for stoichiometric water splitting.
Kazuhiko Maeda—Research Fellow of the Japan Society for the Promotion of Science (JSPS). 相似文献
12.
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
13.
Kazuhiko MaedaAuthor vitae 《Journal of Photochemistry and Photobiology, C: Photochemistry Reviews》2011,12(4):237-268
Overall water splitting to produce H2 and O2 over a semiconductor photocatalyst using solar energy is a promising process for the large-scale production of clean, recyclable H2. Numerous attempts have been made to develop photocatalysts that function under visible-light irradiation to efficiently utilize solar energy. In general, overall water splitting over a photocatalyst particle can be achieved by modifying the photocatalyst with a suitable cocatalyst to provide an active redox site. Therefore, the development of active photocatalytic materials has relied on both photocatalysts and cocatalysts. This review article describes the historical development of water-splitting photocatalysts. 相似文献
14.
Likuan Zhao Yuhang Qi Lizhu Song Shangbo Ning Shuxin Ouyang Hua Xu Jinhua Ye 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(23):7790-7794
Hydrogen production from coal gasification provides a cleaning approach to convert coal resource into chemical energy, but the key procedures of coal gasification and thermal catalytic water–gas shift (WGS) reaction in this energy technology still suffer from high energy cost. We herein propose adopting a solar–driven WGS process instead of traditional thermal catalysis, with the aim of greatly decreasing the energy consumption. Under light irradiation, the CuOx/Al2O3 delivers excellent catalytic activity (122 μmol gcat?1 s?1 of H2 evolution and >95 % of CO conversion) which is even more efficient than noble‐metal‐based catalysts (Au/Al2O3 and Pt/Al2O3). Importantly, this solar‐driven WGS process costs no electric/thermal power but attains 1.1 % of light‐to‐energy storage. The attractive performance of the solar‐driven WGS reaction over CuOx/Al2O3 can be attributed to the combined photothermocatalysis and photocatalysis. 相似文献
15.
Jian Bao Wenjun Liu Junfeng Xie Li Xu Meili Guan Fengcai Lei Yan Zhao Yunpeng Huang Jiexiang Xia Huaming Li 《化学:亚洲杂志》2019,14(3):480-485
Developing highly active, stable and robust electrocatalysts based on earth‐abundant elements for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is important for many renewable energy conversion processes. Herein, NixCo3‐xO4 nanoneedle arrays grown on 3D porous nickel foam (NF) was synthesized as a bifunctional electrocatalyst with OER and HER activity for full water splitting. Benefiting from the advantageous structure, the composite exhibits superior OER activity with an overpotential of 320 mV achieving the current density of 10 mA cm?2. An exceptional HER activity is also acquired with an overpotential of 170 mV at the current density of 10 mA cm?2. Furthermore, the catalyst also shows the superior activity and stability for 20 h when used in the overall water splitting cell. Thus, the hierarchical 3D structure composed of the 1D nanoneedle structure in NixCo3‐xO4/NF represents an avenue to design and develop highly active and bifunctional electrocatalysts for promising energy conversion. 相似文献
16.
The following complex oxynitride perovskites have been prepared: LaMg1/3Ta2/3O2N, LaMg1/2Ta1/2O5/2N1/2, and BaSc0.05Ta0.95O2.1N0.9. Synchrotron X-ray powder diffraction analyses show that LaMg1/3Ta2/3O2N and LaMg1/2Ta1/2O5/2N1/2 are isostructural to the oxide La2Mg(Mg1/3Ta2/3)O6 (space group P21/n), whereas BaSc0.05Ta0.95O2.1N0.9 has a simple cubic symmetry similarly to BaTaO2N. The orderings of octahedral cations are markedly diminished in the above oxynitrides, as compared with the related oxides such as La2Mg(Mg1/3Ta2/3)O6 and Ba2ScTaO6. The optical band gaps are similar for the homologous compositions, LaMg1/3Ta2/3O2N, LaMg1/2Ta1/2O5/2N1/2 and LaTaON2 (1.9 eV), and BaSc0.05Ta0.95O2.1N0.9 and BaTaO2N (1.8 eV), while the absorption edges become broader for the complex derivatives. As revealed from the impedance spectroscopic analysis, the oxynitrides have clearly different dielectric components from those of comparable oxides containing Ta5+. Impedance spectroscopy reveals interesting capacitor geometry in BaSc0.05Ta0.95O2.1N0.9 in which the semiconducting oxynitride grains are separated by insulating secondary phases. Most notably BaSc0.05Ta0.95O2.1N0.9 has a bulk component with a high relative permittivity (κ=7300) and the grain boundary component with an even higher κ. 相似文献
17.
Two approaches for harvesting solar light energy effectively using oxide semiconductor materials are introduced. The one is
water splitting using new types of oxide semiconductor photocatalyst systems. By Na2CO3 addition method, it was firstly demonstrated that water is decomposed to H2 and O2 steadily and stoichiometrically using NiO/TiO2 photocatalyst under the solar light. A new two-step water splitting system using photocatalysis is also introduced. The other
is dyesensitized oxide semiconductor solar cells in order to convert visible light energy to electricity. Combinations of
various types of oxide semiconductors and organic dyes, such as Eosin-Y, suggests the appearance of promising and cheap solar
cells. 相似文献
18.
Decoupling Hydrogen and Oxygen Production in Acidic Water Electrolysis Using a Polytriphenylamine‐Based Battery Electrode
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Yuanyuan Ma Xiaoli Dong Prof. Yonggang Wang Prof. Yongyao Xia 《Angewandte Chemie (International ed. in English)》2018,57(11):2904-2908
Hydrogen production through water splitting is considered a promising approach for solar energy harvesting. However, the variable and intermittent nature of solar energy and the co‐production of H2 and O2 significantly reduce the flexibility of this approach, increasing the costs of its use in practical applications. Herein, using the reversible n‐type doping/de‐doping reaction of the solid‐state polytriphenylamine‐based battery electrode, we decouple the H2 and O2 production in acid water electrolysis. In this architecture, the H2 and O2 production occur at different times, which eliminates the issue of gas mixing and adapts to the variable and intermittent nature of solar energy, facilitating the conversion of solar energy to hydrogen (STH). Furthermore, for the first time, we demonstrate a membrane‐free solar water splitting through commercial photovoltaics and the decoupled acid water electrolysis, which potentially paves the way for a new approach for solar water splitting. 相似文献
19.
Min Wang Jia-Qi Wang Cong Xi Chuan-Qi Cheng Cheng-Qin Zou Rui Zhang Ya-Meng Xie Zhong-Lu Guo Prof. Cheng-Chun Tang Dr. Cun-Ku Dong Prof. Yong-Jun Chen Prof. Xi-Wen Du 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(28):11607-11612
Developing highly efficient and low-cost photocatalysts for overall water splitting has long been a pursuit for converting solar power into clean hydrogen energy. Herein, we demonstrate that a nonstoichiometric nickel–cobalt double hydroxide can achieve overall water splitting by itself upon solar light irradiation, avoiding the consumption of noble-metal co-catalysts. We employed an intensive laser to ablate a NiCo alloy target immersed in alkaline solution, and produced so-called L-NiCo nanosheets with a nonstoichiometric composition and O2−/Co3+ ions exposed on the surface. The nonstoichiometric composition broadens the band gap, while O2− and Co3+ ions boost hydrogen and oxygen evolution, respectively. As such, the photocatalyst achieves a H2 evolution rate of 1.7 μmol h−1 under AM 1.5G sunlight irradiation and an apparent quantum yield (AQE) of 1.38 % at 380 nm. 相似文献
20.
Dr. Angel T. Garcia-Esparza Dr. Tatsuya Shinagawa Dr. Samy Ould-Chikh Muhammad Qureshi Dr. Xuyuan Peng Dr. Nini Wei Dr. Dalaver H. Anjum Dr. Alain Clo Dr. Tsu-Chien Weng Dr. Dennis Nordlund Dr. Dimosthenis Sokaras Prof. Jun Kubota Prof. Kazunari Domen Prof. Kazuhiro Takanabe 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(21):5874-5878
For overall water-splitting systems, it is essential to establish O2-insensitive cathodes that allow cogeneration of H2 and O2. An acid-tolerant electrocatalyst is described, which employs a Mo-coating on a metal surface to achieve selective H2 evolution in the presence of O2. In operando X-ray absorption spectroscopy identified reduced Pt covered with an amorphous molybdenum oxyhydroxide hydrate with a local structural order composed of polyanionic trimeric units of molybdenum(IV). The Mo layer likely hinders O2 gas permeation, impeding contact with active Pt. Photocatalytic overall water splitting proceeded using MoOx/Pt/SrTiO3 with inhibited water formation from H2 and O2, which is the prevailing back reaction on the bare Pt/SrTiO3 photocatalyst. The Mo coating was stable in acidic media for multiple hours of overall water splitting by membraneless electrolysis and photocatalysis. 相似文献