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Cao-Thang Dinh, Thomas Burdyny, Md Golam Kibria, Ali Seifitokaldani, Christine M Gabardo, F Pelayo García de Arquer, Amirreza Kiani, Jonathan P Edwards, Phil De Luna, Oleksandr S Bushuyev, Chengqin Zou, Rafael Quintero-Bermudez, Yuanjie Pang, David Sinton, Edward H Sargent
Carbon dioxide (CO2 ) electroreduction could provide a useful source of ethylene, but low conversion efficiency, low production rates, and low catalyst stability limit current systems. Here we report that a copper electrocatalyst at an abrupt reaction interface in an alkaline electrolyte reduces CO2 to ethylene with 70% faradaic efficiency at a potential of -0.55 volts versus a reversible hydrogen electrode (RHE). Hydroxide ions on or near the copper surface lower the CO2 reduction and carbon monoxide (CO)-CO coupling activation energy barriers; as a result, onset of ethylene evolution at -0...
May 18, 2018: Science
Diana Mesquita Fernandes, Hugo C Novais, Revathi R Bacsa, Philippe Serp, Belén Bachiller-Baeza, Inmaculada Rodriguez-Ramos, Antonio Guerrero-Ruiz, Cristina Freire
The oxygen reduction reaction (ORR) has a crucial function as the cathode reaction in energy-converting systems, such as fuel cells (FCs), which contributes to a sustainable energy supply. However, the current use of precious Pt-based electrocatalysts (ECs) is a major drawback for the economic viability of fuel cells. Hence, it is urgent to develop cost-effective and efficient electrocatalysts (ECs) without noble metals to substitute the Pt-based ECs. Herein, we report the preparation and application as ORR electrocatalysts of four new nanocomposites based on sandwich-type phosphotungstate [(TBA)7H3[Co4(H2O)2(PW9O34)2] (TBA-Co4(PW9)2) immobilized onto different carbon nanomaterials (single-walled carbon nanotubes (SWCNT), graphene flakes (GF), carbon nanotubes doped with nitrogen (N-CNT) and nitrogen-doped few layer graphene (N-FLG))...
May 16, 2018: Langmuir: the ACS Journal of Surfaces and Colloids
Feng Li, Jing Li, Jie Zhang, Lili Gao, Xuefeng Long, Yiping Hu, Shuwen Li, Jun Jin, Jiantai Ma
The photoelectrochemical (PEC) water splitting efficiency of hematite-based photoanode is still far from the theoretical value due to its poor surface reaction kinetics and high density of surface trapping states. To solve these drawbacks, a photoanode consisting of NiO nanoparticles anchored on a gradient P-doped α-Fe2O3 nanorod (NR) array (NiO/P-α-Fe2O3) was fabricated to achieve optimal light absorption and charge separation, and rapid surface reaction kinetic. Specifically, the photoanode with the NR arrays structure allowed high mass transport rate to be achieved while the P-doping effectively decreased surface trapping sites and improved the electrical conductivity of α-Fe2O3...
May 16, 2018: ChemSusChem
Christopher P Muzzillo, W Ellis Klein, Zhen Li, Alexander Daniel DeAngelis, Kimberly Horsley, Kai Zhu, Nicolas Gaillard
Photoelectrochemical (PEC) water-splitting is an elegant method of converting sunlight and water into H2 fuel. To be commercially advantageous, PEC devices must become cheaper, more efficient and much more durable. This work examines low-cost polycrystalline chalcopyrite films, which are successful as photovoltaic absorbers, for application as PEC absorbers. In particular, Cu-Ga-Se films with wide band gaps can be employed as top cell photocathodes in tandem devices as a realistic route to high efficiencies...
May 16, 2018: ACS Applied Materials & Interfaces
Kakali Maiti, Jayaraman Balamurugan, Shaik Gouse Peera, Prof Nam Hoon Kim, Joong-Hee Lee
Development of highly active and durable catalysts for oxygen reduction reaction (ORR) alternative to Pt-based catalyst is an essential topic of interest in research community but challenging task. Here, we have developed a new type of face-centered tetragonal (fct) PdFe alloy nanoparticles encapsulated Pd (fct-PdFe@Pd) anchored onto nitrogen-doped graphene (NG). This core-shell fct-PdFe@Pd@NG hybrid is fabricated by facile and cost-effective technique. The effect of temperature on the transformation of face-centered cubic (fcc) to fct structure and their effect on ORR activity are systematically investigated...
May 14, 2018: ACS Applied Materials & Interfaces
S Gonen, O Lori, G Cohen-Taguri, L Elbaz
Owing to their unique chemistry and physical properties, metal-organic frameworks (MOFs) are an interesting class of materials which can be utilized for a wide array of applications. MOFs have been proposed to be used as catalysts for fuel cells, but their low intrinsic electronic conductivity hampered their utilization as is. In this work, we present the synthesis and application of MOF-based precious-metal-group-free (PGM-free) catalysts for oxygen reduction based on a unique metal-organic framework-carbon composite material...
May 14, 2018: Nanoscale
Jingjing Xu, Ruifang Zhang, Shiyao Lu, Huan Liu, Zhaoyang Li, Xinyu Zhang, Shujiang Ding
A facile and ultrafast microwave-assisted thermolysis approach has been adopted to synthesize hierarchical nitrogen-doped carbon within a very short time. The precursor PANI@carbon felt composite was pyrolyzed in microwave oven for different time (10s, 20s, 30s, 40s, 50s) and denoted as NC-X (X=10, 20, 30, 40, 50). As for NC-30, nitrogen-doping content is obtained up to 3.62 at.% with striking enrichment of pyridinic N as high as 45 % of the total nitrogen content. Raman analysis indicates the extent graphitization level for the resultant NC-30 and the relative intensity ID/IG was 1...
May 11, 2018: Nanotechnology
Xiaoping Zhang, Rong-Mei Kong, Huitong Du, Lian Xia, Fengli Qu
The development of a sustainable route to ammonia production is one of the most attractive targets in chemistry. The primary method of ammonia production, Haber-Bosch process, can bring about excessive consumption of fossil fuels and large CO2 emission. In this communication, we develop a VN nanowire array on carbon cloth (VN/CC) as a high-performance catalyst for the nitrogen reduction reaction (NRR) under ambient conditions. Such an electrocatalyst achieves high ammonia yield (2.48 × 10-10 mol-1 s-1 cm-2) and faradaic efficiency (3...
May 8, 2018: Chemical Communications: Chem Comm
L J Yang, Y Q Deng, X F Zhang, H Liu, W J Zhou
Acid-stable and efficient hydrogen evolution reaction (HER) catalysts have been widely reported. However, achieving full water splitting catalysis in acidic electrolytes is still an urgent task due to the lack of efficient, abundant and acid-stable oxygen evolution reaction (OER) catalysts. This rationally designed MoSe2 nanosheet/MoO2 nanobelt/carbon nanotube membrane (MoSe2 NS/MoO2 NB/CNT-M) is composed of highly conductive CNTs and hierarchical MoSe2 nanosheets on MoO2 nanobelts, and due to its flexible three-dimensional (3D) electrodes, possesses an open architecture for rapid ion/electron diffusion, maximising the exposure of its active sites...
May 8, 2018: Nanoscale
Nor Zuliana Yusof, Siti Salwa Abd Gani, Zafarizal Aldrin Azizul Hasan, Zainab Idris
Many types of phytochemicals have been found to be present in oil palm leaf and could potentially be used as functional ingredients for skincare product. However, as of today, there is no published report on hazard identification and safety assessment of oil palm ( Elaeis guineensis) leaf extract (OPLE), particularly on skin and eye irritation. In this study, potential hazard of OPLE on skin and eye irritation was evaluated as an initial step to the safety assessment of OPLE. In vitro cell viability study of OPLE on normal human dermal fibroblasts showed that OPLE was nontoxic to the cells with percentage viability more than 90% after 24 and 48 hours of incubation...
January 1, 2018: International Journal of Toxicology
Qiheng Li, Wenxing Chen, Hai Xiao, Yue Gong, Zhi Li, Lirong Zheng, Xusheng Zheng, Wensheng Yan, Weng-Chon Cheong, Rongan Shen, Ninghua Fu, Lin Gu, Zhongbin Zhuang, Chen Chen, Dingsheng Wang, Qing Peng, Jun Li, Yadong Li
Heteroatom-doped Fe-NC catalyst has emerged as one of the most promising candidates to replace noble metal-based catalysts for highly efficient oxygen reduction reaction (ORR). However, delicate controls over their structure parameters to optimize the catalytic efficiency and molecular-level understandings of the catalytic mechanism are still challenging. Herein, a novel pyrrole-thiophene copolymer pyrolysis strategy to synthesize Fe-isolated single atoms on sulfur and nitrogen-codoped carbon (Fe-ISA/SNC) with controllable S, N doping is rationally designed...
May 4, 2018: Advanced Materials
Jinjin Ban, Guancheng Xu, Li Zhang, Gui Xu, Lijuan Yang, Zhipeng Sun, Dianzeng Jia
Cobalt-based, nitrogen-doped porous carbon materials with in situ grown carbon nanotubes (CNTs) were synthesized by the facile carbonization of porous 3D Bio-MOF-11 [Co2(ad)2(CH3COO)2]·2DMF·0.5H2O (ad = adenine). Co-N/PC@CNT-Ts inherit the octahedral shape from the precursor, and have a porous structure with in situ grown CNTs catalyzed by Co particles. Co-N/PC@CNT-T materials have excellent activities as bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in 0...
May 2, 2018: Nanoscale
Shouli Bai, Jingchao Liu, Meng Cui, Ruixian Luo, Jing He, Aifan Chen
A Cu2O/BiVO4 p-n heterojunction based photoanode in photoelectrochemical (PEC) water splitting is fabricated by a two-step electrodeposition method on an FTO substrate followed by annealing treatment. The structures and properties of the samples are characterized by XRD, FESEM, HRTEM, XPS and UV-visible spectra. The photoelectrochemical activity of the photoanode in water oxidation has been investigated and measured in a three electrode quartz cell system; the obtained maximum photocurrent density of 1.72 mA cm-2 at 1...
May 2, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
Hui Li, Peng Wen, Adam Hoxie, Chaochao Dun, Shiba Adhikari, Qi Li, Chang Lu, Dominique Itanze, Lin Jiang, David L Carroll, Abdou Lachgar, Yejun Qiu, Scott Geyer
Colloidal semiconductor quantum dots-based (CQD) photocathodes for solar-driven hydrogen evolution have attracted significant attention due to their tunable size, nanostructured morphology, crystalline orientation, and band-gap. Here, we report a thin film heterojunction photocathode composed of organic PEDOT:PSS as a hole transport layer, CdSe CQDs as a semiconductor light absorber, and conformal Pt layer deposited by atomic layer deposition (ALD) serving as both a passivation layer and cocatalyst for hydrogen evolution...
April 30, 2018: ACS Applied Materials & Interfaces
Yong Na, Peicheng Wei
A WO3/TiO2 heterojunction photoanode was prepared by in-situ growth of WO3 on a mesoporous TiO2 electrode. The photoinduced charge transfer properties and charge separation improvement in this kind of type-II heterojunction were characterized by transient surface photovoltage spectra. By using sulfite oxidation as a hole scavenger, we demonstrated that 72% of the photo-generated holes are reaching the surface of the photoanode, but the efficiency of hole injection (ηox) into the electrolyte was only 48%. For the first time, a nickel porphyrin (NiTCPP) was incorporated as a water oxidation catalyst into the WO3/TiO2 heterojunction photoanode, which promoted the value of ηox to be 81%...
April 26, 2018: ChemSusChem
Chang Liu, Pengcheng Wu, Keliang Wu, Guihua Meng, Jianning Wu, Juan Hou, Zhiyong Liu, Xuhong Guo
In this work, a CoPi-decorated type II heterojunction composed of one-dimensional (1D) ZnO nanorod arrays (NRAs) coated with two-dimensional (2D) carbon nitride (g-C3N4) was successfully prepared and used as photoanode. CoPi has been speculated to be a mixture of amorphous compound and two cobalt-based compounds: Co3(PO3)6·14H2O and Co(H2PO2)2·6H2O. The advanced bi-functional CoPi acts like a shelter, effectively inhibiting the photocorrosion of CNNS/ZnO NRAs and providing a faster hole transfer channel. Synergistic effects at the interface of the heterojunction efficiently improve the separation of charge carriers from photoexcited g-C3N4 nanosheets to the ZnO nanorods...
April 27, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
Marc Robert, Tai-Chu Lau, Min Wang, Lingjing Chen
Associating a molecular earth-abundant metal based catalyst to a carbon based nanomaterial is a promising approach for the production of solar fuels from CO2. Upon appending a Co(II) quaterpyridine complex [Co(qpy)]2+ at the surface of multi-walled carbon nanotubes, CO2 conversion into CO was realized in water at pH 7.3 with 100% catalytic selectivity and 100% Faradaic efficiency, at low catalyst loading and reduced overpotential. While a current density of 0.94 mA cm-2 was reached at -0.35 V vs. RHE (240 mV overpotential), 9...
April 25, 2018: Angewandte Chemie
Paula Perez-Rodriguez, Drialys Cardenas-Morcoso, Ibadillah A Digdaya, Andrea Mangel Raventos, Paul Procel, Olindo Isabella, Sixto Gimenez, Miro Zeman, Wilson A Smith, Arno H M Smets
Amorphous silicon carbide (a-SiC:H) is a promising material for photoelectrochemical (PEC) water splitting due to its relatively small bandgap energy and high chemical and optoelectrical stability. This work studies the interplay between charge carrier separation and collection, and their injection into the electrolyte, when modifying the semiconductor/electrolyte interface. By introducing an n-doped nanocrystaline silicon oxide (nc-SiOx:H) layer into a p/i amorphous silicon carbide (a-SiC:H) photocathode, the photovoltage and photocurrent of the device can be significantly improved, reaching values higher than 0...
April 25, 2018: ChemSusChem
Chiung-Yueh Hsu, Nicolas Lecland, Valérie Pendaries, Cécile Viodé, Daniel Redoulès, Carle Paul, Andreas Merdes, Michel Simon, Christiane Bierkamp
BACKGROUND: A variety of human skin disorders is characterized by defects in the epidermal barrier, leading to dehydration, itchiness, and rashes. Previously published literature suggests that microtubule stabilization at the cortex of differentiating keratinocytes is necessary for the formation of the epidermal barrier. OBJECTIVES: We tested whether stabilization of microtubules with paclitaxel or epothilone B can repair barrier defects that were experimentally induced in three-dimensional culture models of epidermis...
April 18, 2018: Journal of Dermatological Science
Chencheng Hu, Zhengran Yi, Wanxin She, Juan Wang, Junwu Xiao, Shuai Wang
We successfully design and construct urchin-like non-precious-metal bifunctional oxygen electrocatalysts via a two-step pyrolysis process, where nitrogen, sulfur co-doped carbon nanotube frameworks are grafted onto mesoporous cobalt sulfide/nitrogen, sulfur co-doped carbon spheres. The urchin-like structure grants large electrochemically active area, good electron and mass transfer capability, as well as excellent structural stability. Nitrogen, sulfur co-doped carbon can synergistically enhance the catalytic activity of cobalt sulfide sites, and also contribute to the exposure of heteroatom-induced active sites, such as, pyridinic N, graphitic N, and C-S-C...
April 13, 2018: Journal of Colloid and Interface Science
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