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26 Dec 02:01

Design principles for maximizing photovoltage in metal-oxide-protected water-splitting photoanodes

by Andrew G. Scheuermann

Nature Materials 15, 99 (2016). doi:10.1038/nmat4451

Authors: Andrew G. Scheuermann, John P. Lawrence, Kyle W. Kemp, T. Ito, Adrian Walsh, Christopher E. D. Chidsey, Paul K. Hurley & Paul C. McIntyre

26 Dec 01:54

Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies

by Hong Li
Shunji_xie

氧缺陷提的蛮多,硫缺陷。。。

Nature Materials 15, 48 (2016). doi:10.1038/nmat4465

Authors: Hong Li, Charlie Tsai, Ai Leen Koh, Lili Cai, Alex W. Contryman, Alex H. Fragapane, Jiheng Zhao, Hyun Soon Han, Hari C. Manoharan, Frank Abild-Pedersen, Jens K. Nørskov & Xiaolin Zheng

As a promising non-precious catalyst for the hydrogen evolution reaction (HER; refs ,,,,), molybdenum disulphide (MoS2) is known to contain active edge sites and an inert basal plane. Activating the MoS2 basal plane could further enhance its HER activity but is not often a strategy for doing so. Herein, we report the first activation and optimization of the basal plane of monolayer 2H-MoS2 for HER by introducing sulphur (S) vacancies and strain. Our theoretical and experimental results show that the S-vacancies are new catalytic sites in the basal plane, where gap states around the Fermi level allow hydrogen to bind directly to exposed Mo atoms. The hydrogen adsorption free energy (ΔGH) can be further manipulated by straining the surface with S-vacancies, which fine-tunes the catalytic activity. Proper combinations of S-vacancy and strain yield the optimal ΔGH = 0 eV, which allows us to achieve the highest intrinsic HER activity among molybdenum-sulphide-based catalysts.

26 Dec 01:45

Water reduction by a p-GaInP2 photoelectrode stabilized by an amorphous TiO2 coating and a molecular cobalt catalyst

by Jing Gu

Nature Materials. doi:10.1038/nmat4511

Authors: Jing Gu, Yong Yan, James L. Young, K. Xerxes Steirer, Nathan R. Neale & John A. Turner

15 Dec 00:35

Strategies for the Conversion of Lignin to High-Value Polymeric Materials: Review and Perspective

by Brianna M. Upton and Andrea M. Kasko

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Chemical Reviews
DOI: 10.1021/acs.chemrev.5b00345
14 Dec 01:19

[Report] CO2 capture from humid flue gases and humid atmosphere using a microporous coppersilicate

by Shuvo Jit Datta
Capturing CO2 from humid flue gases and atmosphere with porous materials remains costly because prior dehydration of the gases is required. A large number of microporous materials with physical adsorption capacity have been developed as CO2-capturing materials. However, most of them suffer from CO2 sorption capacity reduction or structure decomposition that is caused by co-adsorbed H2O when exposed to humid flue gases and atmosphere. We report a highly stable microporous coppersilicate. It has H2O-specific and CO2-specific adsorption sites but does not have H2O/CO2-sharing sites. Therefore, it readily adsorbs both H2O and CO2 from the humid flue gases and atmosphere, but the adsorbing H2O does not interfere with the adsorption of CO2. It is also highly stable after adsorption of H2O and CO2 because it was synthesized hydrothermally. Authors: Shuvo Jit Datta, Chutharat Khumnoon, Zhen Hao Lee, Won Kyung Moon, Son Docao, Thanh Huu Nguyen, In Chul Hwang, Dohyun Moon, Peter Oleynikov, Osamu Terasaki, Kyung Byung Yoon
14 Dec 00:52

[Report] Semiconductor interfacial carrier dynamics via photoinduced electric fields

by Ye Yang
Solar photoconversion in semiconductors is driven by charge separation at the interface of the semiconductor and contacting layers. Here we demonstrate that time-resolved photoinduced reflectance from a semiconductor captures interfacial carrier dynamics. We applied this transient photoreflectance method to study charge transfer at p-type gallium-indium phosphide (p-GaInP2) interfaces critically important to solar-driven water splitting. We monitored the formation and decay of transient electric fields that form upon photoexcitation within bare p-GaInP2, p-GaInP2/platinum (Pt), and p-GaInP2/amorphous titania (TiO2) interfaces. The data show that a field at both the p-GaInP2/Pt and p-GaInP2/TiO2 interfaces drives charge separation. Additionally, the charge recombination rate at the p-GaInP2/TiO2 interface is greatly reduced owing to its p-n nature, compared with the Schottky nature of the p-GaInP2/Pt interface. Authors: Ye Yang, Jing Gu, James L. Young, Elisa M. Miller, John A. Turner, Nathan R. Neale, Matthew C. Beard
14 Dec 00:50

[Report] Electron-hole pair excitation determines the mechanism of hydrogen atom adsorption

by Oliver Bünermann
How much translational energy atoms and molecules lose in collisions at surfaces determines whether they adsorb or scatter. The fact that hydrogen (H) atoms stick to metal surfaces poses a basic question. Momentum and energy conservation demands that the light H atom cannot efficiently transfer its energy to the heavier atoms of the solid in a binary collision. How then do H atoms efficiently stick to metal surfaces? We show through experiments that H-atom collisions at an insulating surface (an adsorbed xenon layer on a gold single-crystal surface) are indeed nearly elastic, following the predictions of energy and momentum conservation. In contrast, H-atom collisions with the bare gold surface exhibit a large loss of translational energy that can be reproduced by an atomic-level simulation describing electron-hole pair excitation. Authors: Oliver Bünermann, Hongyan Jiang, Yvonne Dorenkamp, Alexander Kandratsenka, Svenja M. Janke, Daniel J. Auerbach, Alec M. Wodtke
11 Dec 00:39

An electrodeposited inhomogeneous metal–insulator–semiconductor junction for efficient photoelectrochemical water oxidation

by James C. Hill

Nature Materials 14, 1150 (2015). doi:10.1038/nmat4408

Authors: James C. Hill, Alan T. Landers & Jay A. Switzer

11 Dec 00:38

Efficient hydrogen evolution catalysis using ternary pyrite-type cobalt phosphosulphide

by Miguel Cabán-Acevedo

Nature Materials 14, 1245 (2015). doi:10.1038/nmat4410

Authors: Miguel Cabán-Acevedo, Michael L. Stone, J. R. Schmidt, Joseph G. Thomas, Qi Ding, Hung-Chih Chang, Meng-Lin Tsai, Jr-Hau He & Song Jin

10 Dec 00:36

Plasma Catalysis: Synergistic Effects at the Nanoscale

by Erik C. Neyts, Kostya (Ken) Ostrikov, Mahendra K. Sunkara and Annemie Bogaerts

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Chemical Reviews
DOI: 10.1021/acs.chemrev.5b00362
21 Nov 02:04

Iron sensitizer converts light to electrons with 92% yield

by Tobias C. B. Harlang

Nature Chemistry. doi:10.1038/nchem.2365

Authors: Tobias C. B. Harlang, Yizhu Liu, Olga Gordivska, Lisa A. Fredin, Carlito S. Ponseca, Ping Huang, Pavel Chábera, Kasper S. Kjaer, Helena Mateos, Jens Uhlig, Reiner Lomoth, Reine Wallenberg, Stenbjörn Styring, Petter Persson, Villy Sundström & Kenneth Wärnmark

Using iron instead of the scarce ruthenium in light-harvesting complexes is challenging because iron complexes generally have short-lived excited states. Now an iron complex has been developed that has a long-lived excited state, which can lead to photo-induced electron injection into nanoporous TiO2 with a yield of 92%.

21 Nov 01:57

Electrocatalysis: Powered by porphyrin packing

by Idan Hod

Nature Materials 14, 1192 (2015). doi:10.1038/nmat4494

Authors: Idan Hod, Omar K. Farha & Joseph T. Hupp

Self-assembling covalent organic frameworks can boost electrode performance for the catalytic reduction of carbon dioxide.

13 Nov 10:24

Current Issues in Molecular Catalysis Illustrated by Iron Porphyrins as Catalysts of the CO2-to-CO Electrochemical Conversion

by Cyrille Costentin, Marc Robert and Jean-Michel Savéant

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Accounts of Chemical Research
DOI: 10.1021/acs.accounts.5b00262
13 Nov 10:14

Electrochemical Synthesis of Photoelectrodes and Catalysts for Use in Solar Water Splitting

by Donghyeon Kang, Tae Woo Kim, Stephen R. Kubota, Allison C. Cardiel, Hyun Gil Cha and Kyoung-Shin Choi

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Chemical Reviews
DOI: 10.1021/acs.chemrev.5b00498
13 Nov 10:14

Oxidative Coupling between Two Hydrocarbons: An Update of Recent C–H Functionalizations

by Chao Liu, Jiwen Yuan, Meng Gao, Shan Tang, Wu Li, Renyi Shi and Aiwen Lei

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Chemical Reviews
DOI: 10.1021/cr500431s
16 Sep 00:31

An electrodeposited inhomogeneous metal–insulator–semiconductor junction for efficient photoelectrochemical water oxidation

by James C. Hill

Nature Materials. doi:10.1038/nmat4408

Authors: James C. Hill, Alan T. Landers & Jay A. Switzer

26 Jul 02:22

Light Induced Carbon Dioxide Reduction by Water at Binuclear ZrOCoII Unit Coupled to Ir Oxide Nanocluster Catalyst

by Wooyul Kim, Guangbi Yuan, Beth Anne McClure and Heinz Frei

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Journal of the American Chemical Society
DOI: 10.1021/ja504753g
07 Jul 01:06

Ultrafast Charge Carrier Recombination and Trapping in Hematite Photoanodes under Applied Bias

by Stephanie R Pendlebury, Xiuli Wang, Florian Le Formal, Maurin Cornuz, Andreas Kafizas, S. David Tilley, Michael Grätzel and James R Durrant

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Journal of the American Chemical Society
DOI: 10.1021/ja504473e
04 Jun 04:02

A Tantalum Nitride Photoanode Modified with a Hole-Storage Layer for Highly Stable Solar Water Splitting

by Guiji Liu, Jingying Shi, Fuxiang Zhang, Zheng Chen, Jingfeng Han, Chunmei Ding, Shanshan Chen, Zhiliang Wang, Hongxian Han, Can Li

Abstract

Photoelectrochemical (PEC) water splitting is an ideal approach for renewable solar fuel production. One of the major problems is that narrow bandgap semiconductors, such as tantalum nitride, though possessing desirable band alignment for water splitting, suffer from poor photostability for water oxidation. For the first time it is shown that the presence of a ferrihydrite layer permits sustainable water oxidation at the tantalum nitride photoanode for at least 6 h with a benchmark photocurrent over 5 mA cm−2, whereas the bare photoanode rapidly degrades within minutes. The remarkably enhanced photostability stems from the ferrihydrite, which acts as a hole-storage layer. Furthermore, this work demonstrates that it can be a general strategy for protecting narrow bandgap semiconductors against photocorrosion in solar water splitting.

Thumbnail image of graphical abstract

The presence of a ferrihydrite layer allows stable water oxidation at the Co3O4/ferrihydrite/Ta3N5 photoanode for at least 6 h. This is the Ta3N5-based photoanode that is the most durable against photocorrosion reported to date. The role of the ferrihydrite layer is a hole-storage layer, increasing the hole-storage capacity and suppressing photocorrosion of Ta3N5 electrode.

28 May 01:39

Efficient Reduction of CO2 to CO with High Current Density Using in Situ or ex Situ Prepared Bi-Based Materials

by Jonnathan Medina-Ramos, John L. DiMeglio and Joel Rosenthal

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Journal of the American Chemical Society
DOI: 10.1021/ja501923g
04 May 09:47

Efficient Water Oxidation Using Nanostructured α-Nickel-Hydroxide as an Electrocatalyst

by Minrui Gao, Wenchao Sheng, Zhongbin Zhuang, Qianrong Fang, Shuang Gu, Jun Jiang and Yushan Yan

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Journal of the American Chemical Society
DOI: 10.1021/ja502128j
11 Apr 00:46

Glutathione-Capped Gold Nanoclusters as Photosensitizers. Visible Light-Induced Hydrogen Generation in Neutral Water

by Yong-Siou Chen and Prashant V. Kamat

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Journal of the American Chemical Society
DOI: 10.1021/ja5017365
10 Oct 01:00

Semiconductor Nanowires for Artificial Photosynthesis

by Chong Liu, Neil P. Dasgupta and Peidong Yang

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Chemistry of Materials
DOI: 10.1021/cm4023198
27 Sep 02:34

Inside Back Cover: Asymmetric Diboration of Terminal Alkenes with a Rhodium Catalyst and Subsequent Oxidation: Enantioselective Synthesis of Optically Active 1,2-Diols (Angew. Chem. Int. Ed. 42/2013)

by Mingxue Li, Wenjun Luo, Dapeng Cao, Xin Zhao, Zhaosheng Li, Tao Yu, Zhigang Zou
Thumbnail image of graphical abstract

The highest solar photocurrent among all currently available tantalum nitride (Ta3N5) photoanodes is obtained by oxidation and nitridation of tantalum foils, as described by W. Luo, Z. Zou et al. in their Communication on page 11011 ff. The high photocurrent mainly originates from the facile thermal or mechanical exfoliation of surface recombination centers.

02 Jul 07:06

Energy-Level Matching of Fe(III) Ions Grafted at Surface and Doped in Bulk for Efficient Visible-Light Photocatalysts

by Min Liu, Xiaoqing Qiu, Masahiro Miyauchi and Kazuhito Hashimoto

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Journal of the American Chemical Society
DOI: 10.1021/ja401541k
21 Jun 09:36

Guided Assembly of Tetramolecular G-Quadruplexes

by Liliya A. Yatsunyk, Olivier Piétrement, Delphine Albrecht, Phong Lan Thao Tran, Daniel Renčiuk, Hiroshi Sugiyama, Jean-Michel Arbona, Jean-Pierre Aimé and Jean-Louis Mergny

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ACS Nano
DOI: 10.1021/nn402321g