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101.
Enhancing the Water Splitting Efficiency of Sn‐Doped Hematite Nanoflakes by Flame Annealing 下载免费PDF全文
Dr. Lei Wang Dr. Chong‐Yong Lee Dr. Anca Mazare Dr. Kiyoung Lee Julian Müller Prof. Dr. Erdmann Spiecker Prof. Dr. Patrik Schmuki 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(1):77-82
The effect of flame annealing on the water‐splitting properties of Sn decorated hematite (α‐Fe2O3) nanoflakes has been investigated. It is shown that flame annealing can yield a considerable enhancement in the maximum photocurrent under AM 1.5 (100 mW cm?2) conditions compared to classic furnace annealing treatments. Optimizing the annealing time (10 s at 1000 °C) leads to a photocurrent of 1.1 mA cm?2 at 1.23 V (vs. RHE) with a maximum value 1.6 mA cm?2 at 1.6 V (vs. RHE) in 1 M KOH. The improvement in photocurrent can be attributed to the fast direct heating that maintains the nanoscale morphology, leads to optimized Sn decoration, and minimizes detrimental substrate effects. 相似文献
102.
A Doping Technique that Suppresses Undesirable H2 Evolution Derived from Overall Water Splitting in the Highly Selective Photocatalytic Conversion of CO2 in and by Water 下载免费PDF全文
Prof. Dr. Kentaro Teramura Zheng Wang Dr. Saburo Hosokawa Prof. Dr. Yoshihisa Sakata Prof. Dr. Tsunehiro Tanaka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(32):9906-9909
Photocatalytic conversion of CO2 to reduction products, such as CO, HCOOH, HCHO, CH3OH, and CH4, is one of the most attractive propositions for producing green energy by artificial photosynthesis. Herein, we found that Ga2O3 photocatalysts exhibit high conversion of CO2. Doping of Zn species into Ga2O3 suppresses the H2 evolution derived from overall water splitting and, consequently, Zn‐doped, Ag‐modified Ga2O3 exhibits higher selectivity toward CO evolution than bare, Ag‐modified Ga2O3. We observed stoichiometric amounts of evolved O2 together with CO. Mass spectrometry clarified that the carbon source of the evolved CO is not the residual carbon species on the photocatalyst surface, but the CO2 introduced in the gas phase. Doping of the photocatalyst with Zn is expected to ease the adsorption of CO2 on the catalyst surface. 相似文献
103.
Construction of Shallow Surface States through Light Ni Doping for High‐Efficiency Photocatalytic Hydrogen Production of CdS Nanocrystals 下载免费PDF全文
Shuo Li Lijing Zhang Tengfei Jiang Liping Chen Prof.Dr. Yanhong Lin Prof. Dr. Dejun Wang Prof. Dr. Tengfeng Xie 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(1):311-316
Ni‐doped CdS nanowires were synthesized by a simple one‐step method. X‐ray diffraction, X‐ray photoelectron spectroscopy, and photoluminescence spectroscopy confirmed that light Ni doping can form shallow surface states due to the presence of substitutional Ni ions, and heavy Ni doping can form deep surface states due to the presence of interstitial Ni ions. Surface photovoltage spectroscopy and transient photovoltage measurements revealed that the shallow surface states can prolong the lifetime of the photogenerated charge carriers, whereas the deep surface states lead to recombination of the photogenerated charge carriers. The relationship between different surface states and the photocatalytic performance of CdS nanocrystals are discussed. The enhanced density of shallow surface states due to light Ni doping significantly promotes photocatalytic H2 production. 相似文献
104.
Dr. Jungki Ryu Dong Heon Nam Dr. Sahng Ha Lee Prof.Dr. Chan Beum Park 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(38):12020-12025
Efficient harvesting of unlimited solar energy and its conversion into valuable chemicals is one of the ultimate goals of scientists. With the ever‐increasing concerns about sustainable growth and environmental issues, numerous efforts have been made to develop artificial photosynthetic process for the production of fuels and fine chemicals, thus mimicking natural photosynthesis. Despite the research progress made over the decades, the technology is still in its infancy because of the difficulties in kinetic coupling of whole photocatalytic cycles. Herein, we report a new type of artificial photosynthesis system that can avoid such problems by integrally coupling biocatalytic redox reactions with photocatalytic water splitting. We found that photocatalytic water splitting can be efficiently coupled with biocatalytic redox reactions by using tetracobalt polyoxometalate and Rh‐based organometallic compound as hole and electron scavengers, respectively, for photoexcited [Ru(bpy)3]2+. Based on these results, we could successfully photosynthesize a model chiral compound (L ‐glutamate) using a model redox enzyme (glutamate dehydrogenase) upon in situ photoregeneration of cofactors. 相似文献
105.
Craig J. Richmond Roc Matheu Dr. Albert Poater Dr. Laura Falivene Dr. Jordi Benet‐Buchholz Dr. Xavier Sala Prof. Luigi Cavallo Prof. Antoni Llobet 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(52):17282-17286
Extremely slow and extremely fast new water oxidation catalysts based on the Ru–bda (bda=2,2′‐bipyridine‐6,6′‐dicarboxylate) systems are reported with turnover frequencies in the range of 1 and 900 cycles s?1, respectively. Detailed analyses of the main factors involved in the water oxidation reaction have been carried out and are based on a combination of reactivity tests, electrochemical experiments, and DFT calculations. These analyses give a convergent interpretation that generates a solid understanding of the main factors involved in the water oxidation reaction, which in turn allows the design of catalysts with very low energy barriers in all the steps involved in the water oxidation catalytic cycle. We show that for this type of system π‐stacking interactions are the key factors that influence reactivity and by adequately controlling them we can generate exceptionally fast water oxidation catalysts. 相似文献
106.
Highly Active Electrocatalysis of the Hydrogen Evolution Reaction by Cobalt Phosphide Nanoparticles 下载免费PDF全文
Eric J. Popczun Carlos G. Read Christopher W. Roske Prof. Nathan S. Lewis Prof. Raymond E. Schaak 《Angewandte Chemie (International ed. in English)》2014,53(21):5427-5430
Nanoparticles of cobalt phosphide, CoP, have been prepared and evaluated as electrocatalysts for the hydrogen evolution reaction (HER) under strongly acidic conditions (0.50 M H2SO4, pH 0.3). Uniform, multi‐faceted CoP nanoparticles were synthesized by reacting Co nanoparticles with trioctylphosphine. Electrodes comprised of CoP nanoparticles on a Ti support (2 mg cm?2 mass loading) produced a cathodic current density of 20 mA cm?2 at an overpotential of ?85 mV. The CoP/Ti electrodes were stable over 24 h of sustained hydrogen production in 0.50 M H2SO4. The activity was essentially unchanged after 400 cyclic voltammetric sweeps, suggesting long‐term viability under operating conditions. CoP is therefore amongst the most active, acid‐stable, earth‐abundant HER electrocatalysts reported to date. 相似文献
107.
Large Zero‐Field Splittings of the Ground Spin State Arising from Antisymmetric Exchange Effects in Heterometallic Triangles 下载免费PDF全文
Samantha A. Magee Dr. Stephen Sproules Dr. Anne‐Laure Barra Dr. Grigore A. Timco Nicholas F. Chilton Prof. David Collison Prof. Richard E. P. Winpenny Prof. Eric J. L. McInnes 《Angewandte Chemie (International ed. in English)》2014,53(21):5310-5313
[Ru2Mn(O)(O2CtBu)6(py)3] has an S=5/2 ground state with a very large zero‐field splitting (ZFS) of D=2.9 cm?1, as characterized by EPR spectroscopy at 4–330 GHz. This is far too large to be due to the MnII ion (D <0.2 cm?1), as shown from the {Fe2Mn} analogue, but can be modeled by antisymmetric exchange effects. 相似文献
108.
A Cost‐Effective 3D Hydrogen Evolution Cathode with High Catalytic Activity: FeP Nanowire Array as the Active Phase 下载免费PDF全文
Dr. Ping Jiang Qian Liu Yanhui Liang Dr. Jingqi Tian Prof. Abdullah M. Asiri Prof. Xuping Sun 《Angewandte Chemie (International ed. in English)》2014,53(47):12855-12859
Iron is the cheapest and one of the most abundant transition metals. Natural [FeFe]‐hydrogenases exhibit remarkably high activity in hydrogen evolution, but they suffer from high oxygen sensitivity and difficulty in scale‐up. Herein, an FeP nanowire array was developed on Ti plate (FeP NA/Ti) from its β‐FeOOH NA/Ti precursor through a low‐temperature phosphidation reaction. When applied as self‐supported 3D hydrogen evolution cathode, the FeP NA/Ti electrode shows exceptionally high catalytic activity and good durability, and it only requires overpotentials of 55 and 127 mV to afford current densities of 10 and 100 mA cm2, respectively. The excellent electrocatalytic performance is promising for applications as non‐noble‐metal HER catalyst with a high performance–price ratio in electrochemical water splitting for large‐scale hydrogen fuel production. 相似文献
109.
Photocatalytic Water Oxidation by a Pyrochlore Oxide upon Irradiation with Visible Light: Rhodium Substitution Into Yttrium Titanate 下载免费PDF全文
Borbala Kiss Dr. Christophe Didier Timothy Johnson Dr. Troy D. Manning Dr. Matthew S. Dyer Dr. Alexander J. Cowan Dr. John B. Claridge Prof. James R. Darwent Prof. Matthew J. Rosseinsky 《Angewandte Chemie (International ed. in English)》2014,53(52):14480-14484
A stable visible‐light‐driven photocatalyst (λ≥450 nm) for water oxidation is reported. Rhodium substitution into the pyrochlore Y2Ti2O7 is demonstrated by monitoring Vegard′s law evolution of the unit‐cell parameters with changing rhodium content, to a maximum content of 3 % dopant. Substitution renders the solid solutions visible‐light active. The overall rate of oxygen evolution is comparable to WO3 but with superior light‐harvesting and surface‐area‐normalized turnover rates, making Y2Ti1.94Rh0.06O7 an excellent candidate for use in a Z‐scheme water‐splitting system. 相似文献
110.
Nanocomposites of Tantalum‐Based Pyrochlore and Indium Hydroxide Showing High and Stable Photocatalytic Activities for Overall Water Splitting and Carbon Dioxide Reduction 下载免费PDF全文
Meng‐Chun Hsieh Guan‐Chang Wu Dr. Wei‐Guang Liu Prof. William A. Goddard III Prof. Dr. Chia‐Min Yang 《Angewandte Chemie (International ed. in English)》2014,53(51):14216-14220
Nanocomposites of tantalum‐based pyrochlore nanoparticles and indium hydroxide were prepared by a hydrothermal process for UV‐driven photocatalytic reactions including overall water splitting, hydrogen production from photoreforming of methanol, and CO2 reduction with water to produce CO. The best catalyst was more than 20 times more active than sodium tantalate in overall water splitting and 3 times more active than Degussa P25 TiO2 in CO2 reduction. Moreover, the catalyst was very stable while generating stoichiometric products of H2 (or CO) and O2 throughout long‐term photocatalytic reactions. After the removal of In(OH)3, the pyrochlore nanoparticles remained highly active for H2 production from pure water and aqueous methanol solution. Both experimental studies and density functional theory calculations suggest that the pyrochlore nanoparticles catalyzed the water reduction to produce H2, whereas In(OH)3 was the major active component for water oxidation to produce O2. 相似文献