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Canan Sener, Ali Hussain Motagamwala, David Martin Alonso, James Dumesic
High yields of furfural (>90%) were achieved from xylose dehydration in a sustainable solvent system composed of -valerolactone (GVL), a biomass derived solvent, and water. It is identified that high reaction temperatures (e.g., 498 K) are required to achieve high furfural yield. Additionally, it is shown that the furfural yield at these temperatures is independent of the initial xylose concentration, and high furfural yield is obtained for industrially relevant xylose concentrations (10 wt%). A reaction kinetics model is developed to describe the experimental data obtained with solvent system composed of 80 wt% GVL and 20 wt% water across the range of reaction conditions studied (473 - 523 K, 1-10 mM acid catalyst, 66 - 660 mM xylose concentration)...
May 18, 2018: ChemSusChem
Hongbin Wang, Lijia Liu, Runwei Wang, Xiao Yan, Ziqi Wang, Jiangtao Hu, Haibiao Chen, Shang Jiang, Ling Ni, Hailong Qiu, Haitong Tang, Yingjin Wei, Zongtao Zhang, Qiu Shilun, Feng Pan
LiFePO4@C/rGO hierarchical microspheres with superior electrochemical activity and high tap density were first synthesized using a Fe3+-based single inorganic precursor (LiFePO4OH@RF/GO) obtained from a template-free self-assembly synthesis, following with direct calcination. The synthesis process requires no physical mixing step. The phase transformation path way from tavorite LiFePO4OH to olivine LiFePO4 upon calcination was determined by the in situ high temperature XRD technique. Benefitted from the unique structure of the material, these microspheres can be densely packed together, giving a high tap density of 1...
May 18, 2018: ChemSusChem
Sicong Wang, Zhenyuan Teng, Chengyin Wang, Guoxiu Wang
High activity and stability are crucial for practical electrocatalysts used for reactions in fuel cells, metal-air batteries and water electrolysis including ORR, HER, OER and oxidation reactions of formic acid and alcohols. N-C based electrocatalysts have shown promising prospects for catalyzing these reactions, however, there is no systematic review for strategies toward engineering active and stable N-C based electrocatalysts reported by far. Herein, a comprehensive comparison of recently reported N-C based electrocatalysts regarding both electrocatalytic activity and long-term stability is presented...
May 17, 2018: ChemSusChem
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
Chao-Hsuan Chen, Zhi-Wei Lin, Kuan-Min Huang, Hsin-Fei Meng, Ziyi Ge, Hsiao-Wen Zan, Chih-Yu Chang, Yu-Chiang Chao, Sheng-Fu Horng
Interfacial engineering plays an important role in determining the performance and stability of polymer solar cells (PSCs). In this study, we demonstrate thermally stable highly-efficient PSCs by incorporating solution-processed cathode interfacial layer (CIL), including 4,4'-(((methyl(4-sulphonatobutyl)ammonio) bis(propane-3,1-diyl)) bis(dimethyl-ammoniumdiyl)) bis-(butane-1-sulphonate) (MSAPBS) and polyethylenimine (PEI). For PSCs based on blends of poly [4,8-bis (5-(2-ethyl-hexyl) thiophen-2-yl) benzo [1,2-b;4,5-b'] dithiophene-2,6-diyl-alt-(4-(2-ethylhexyl)-3-fluorothieno[3,4-b]thiophene-2-carboxylate-2,6-diyl)] (PBDTTT-EFT) and [6,6]-phenyl C71-butyric acid methyl ester (PC71BM), the maximum power conversion efficiency (PCE) of inverted PSCs reaches 8...
May 16, 2018: ChemSusChem
Yi Zhou, Shuke Wu, Jiwei Mao, Zhi Li
Production of chemicals from renewable feedstocks has been an important task for sustainable chemical industry. While microbial fermentation has been widely employed to produce many biochemicals, it is still very challenging to access non-natural chemicals. Herein, we developed two methods (biotransformation and fermentation) for the first bio-derived synthesis of benzylamine, a commodity non-natural amine with broad applications. At first, a 9-step artificial enzyme cascade was designed by biocatalytic retrosynthesis analysis and engineered in recombinant E...
May 15, 2018: ChemSusChem
Yuanzhi Zhu, Xifan Chen, Jing Liu, Junfeng Zhang, Danyun Xu, Wenchao Peng, Yang Li, Guoliang Zhang, Fengbao Zhang, Xiaobin Fan
Porous organic polymers (POFs) are promising precursors for developing high performance transition metal-nitrogen-carbon (M-N/C) catalysts towards ORR. But the rational design of POFs precursors remain a great challenge, because of the elusive structural association between the sacrificial POFs and the final M-N/C catalysts. Based on covalent triazine frameworks (CTFs), we developed a series of sulfur-doped Fe-N/C catalysts by selecting six different aromatic nitriles as building blocks. A new mixed solvent of molten FeCl3 and S was used for CTF polymerization, which benefit the formation of Fe-Nx site and make the subsequent pyrolysis process more convenient...
May 15, 2018: ChemSusChem
Xian-Dong Lang, Liang-Nian He
Currently, it still remains a challenge to amplify the spectrum of chemical fixation of CO2, though enormous progresses have been witnessed in this field. In view of the widespread applications of CO in a myriad of industrial carbonylation processes, we proposed an alternative strategy to integrate CO2 reduction to CO and carbonylations with CO ex situ generated, efficiently affording pharmaceutically and agrochemically attractive molecules. As such, CO2 in this study was efficiently reduced by triphenysilane with CsF to CO in a sealed two-chamber reactor; Subsequently, the palladium-catalyzed aminocarbonylation and carbonylative Sonogashira coupling of aryl iodides, rhodium(I)-mediated Pauson-Khand-type reaction proceeded smoothly to furnish the amides, alkynones and bicyclic cyclopentenones, respectively...
May 15, 2018: ChemSusChem
Christian M Pichler, Mohammad Ghith Al-Shaal, Dong Gu, Hrishikesh Joshi, Wirawan Ciptonugroho, Ferdi Schüth
Different ZrO2 supported ruthenium catalysts were prepared and utilized in the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) under base-free conditions. Full conversion of HMF and almost perfect selectivity towards FDCA (97%) were achieved after 16 h, using pure O2 as an oxidant and water as a solvent. The catalytic tests show that the size of the Ru particles is crucial for the catalytic performance and that the utilization of high surface area ZrO2 leads to formation of very small Ru particles...
May 15, 2018: ChemSusChem
Madagonda M Vadiyar, Xudong Liu, Zhibin Ye
In the present work, we demonstrate the synthesis of porous activated carbon (specific surface area, 1,883 m2 g-1), Fe3O4 nanoparticles, and carbon-Fe3O4 nanocomposites using local waste thermocol sheets and rusted iron wires. The resulting carbon, Fe3O4 nanoparticles, and carbon-Fe3O4 composites are used as electrode materials for supercapacitor application. In particular, C-Fe3O4 composite electrodes exhibit a high specific capacitance of 1,375 F g-1 at 1 A g-1 and longer cyclic stability with 98 % of capacitance retention over 10,000 cycles...
May 14, 2018: ChemSusChem
Ziosi Paolo, Paolucci Claudio, Santarelli Francesco, Tabanelli Tommaso, Passeri Sauro, Fabrizio Cavani, Righi Paolo
Here we report about a new process for the synthesis of hydroxytyrosol (3,4-dihydroxyphenylethanol), the most powerful natural antioxidant currently known, by means of a two-step approach. Catechol is first reacted with 2,2 dimethoxyacetaldehyde in basic aqueous medium, to produce the corresponding mandelic derivative with > 90% conversion of the limiting reactant and about 70% selectivity to the desired para-hydroxyalkylated compound. Thereafter, the intermediate is hydrogenated to hydroxytyrosol using a Pd/C catalyst, with total conversion of the mandelic derivative and 68% selectivity...
May 14, 2018: ChemSusChem
Nagarajan Subbiah, Muthusamy K, Lalitha Krishnamoorthy, Siva Prasad Yadavali, Thamizhanban Ayyapillai, Sridharan Vellaisamy, Maheswari C Uma
Bio-based polyesters are well-known biodegradable materials that are frequently used in our daily life, which include food industries and biomedical fields. The journey towards the development of sustainable polymer materials and technology postulate the replacement of traditionally using petrochemical-based monomers, transition metal catalyst, and more intensive purification techniques, which do not agree with the green chemistry principles. This contribution investigates the synthesis of bio-based hydrophilic and hydrophobic oligoesters, which in turn derived from easily accessible monomers of natural resources...
May 11, 2018: ChemSusChem
Sofie Seghers, Thomas S A Heugebaert, Matthias Moens, Jolien Sonck, Joris Thybaut, Chris Victor Stevens
The unique nucleophilic properties of lithiated methoxyallene allow for C-C bond formation with a wide variety of electrophiles, thus introducing an allenic group for further functionalization. This approach has yielded a tremendously broad range of (hetero)cyclic scaffolds, including API precursors. To date, however, its valorization at scale is hampered by the batch synthesis protocol which suffers from serious safety issues. Hence, the attractive heat and mass transfer properties of flow technology were exploited to establish a mesoscale continuous flow route towards lithiated methoxyallene...
May 11, 2018: ChemSusChem
Barbara Kirchner, Johannes Ingenmey, Sascha Gehrke
Hydrogen is often regarded as fuel of the future and we see an increasing demand for the development of anhydrous proton conducting electrolytes to enable fuel cell operation at elevated temperatures exceeding 120~$^\circ$C. Much attention has been directed at protic ionic liquids (PILs) as promising candidate, but in the search for highly conductive systems the possibility of designing Grotthuss diffusion enabled PILs has been widely overlooked. In this work we explored through ab initio molecular dynamics simulations the mechanics of proton transfer mechanism in the equimolar mixture of \textit{N}-methylimidazole and acetic acid...
May 9, 2018: ChemSusChem
Yong Zhang, Seul-Gi Kim, Do-Kyoung Lee, Nam-Gyu Park
High-efficiency perovskite solar cells are generally fabricated by using highly pure (>99.99 %) PbI2 mixed with an organic iodide in polar aprotic solvents. However, the use of such an expensive chemical may impede progress toward large-scale industrial applications. Here, we report on the synthesis of perovskite powders by using inexpensive low-grade (99 %) PbI2 and on the photovoltaic performance of perovskite solar cells prepared from a powder-based single precursor. Pure APbI3 [A=methylammonium (MA) or formamidinium (FA)] perovskite powders were synthesized by treating low-grade PbI2 with MAI or FAI in acetonitrile at ambient temperature...
May 9, 2018: ChemSusChem
Guodong Ding, Ji Su, Cheng Zhang, Kan Tang, Lisha Yang, Hongfei Lin
Conversion of carbon dioxide into value-added chemicals and fuels provides a direct solution to reduce excessive CO2 in the atmosphere. Herein, a novel catalytic reaction system is presented by coupling the dehydrogenation of glucose with the hydrogenation of a CO2 derived salt, ammonium carbonate, in the ethanol-water mixture. For the first time, the hydrogenation of CO2 into formate by glucose has been achieved under ambient conditions. Under the optimal reaction conditions, the highest yield of formate reached ~ 46 %...
May 8, 2018: ChemSusChem
Mobinul Islam, Min-Gi Jeong, Ghulam Ali, In-Hwan Oh, Kyung Yoon Chung, Yang-Kook Sun, Hun-Gi Jung
Boosting the performance of rechargeable Li-ion batteries beyond the state-of-the-art is mandatory toward meeting the future energy requirements of the consumer mass market. The replacement of conventional graphite anodes by conversion-type metal-oxide anodes is one progressive approach toward achieving this goal. Here, a lithium-ion battery consisting of a high-capacity spinel NiMn2O4 anode and a high-voltage spinel LiNi0.5Mn1.5O4 cathode was proposed. Polyhedral-shaped NiMn2O4 powder was prepared from a citrate precursor via the sol-gel method...
May 8, 2018: ChemSusChem
Roland Hischier, Nam Hee Kwon, Jean-Pierre Brog, Katharina M Fromm
We present results of early stage sustainability evaluation of two development strategies for new, nano-scale cathode materials for Li-ion batteries: (i) a new production pathway of existing material (LiCoO2), and (ii) a new nanomaterial (LiMnPO4). Nano-LiCoO2 was synthesized via a single source precursor route at lower temperature with a shorter reaction time, resulting in a smaller grain size and, thereby, a better diffusivity for Li-ions. Nano-LiMnPO4 was synthesized via a wet chemical method. The sustainability potential of these materials has then been investigated (at the laboratory and pilot production scales)...
May 7, 2018: ChemSusChem
David Ferdinand Scholz, Oliver Kröcher, Frédéric Vogel
The deactivation pathways of sulfonated carbon catalysts prepared from different carbons were studied during the aqueous-phase hydrolysis of cellobiose under continuous flow conditions. Sulfonation of carbon materials with a low degree of graphitization, introduced sulfonic acid groups that are partially stable even during prolonged exposure to harsh hydrothermal treatments (180 °C). Physicochemical characterization of hydrothermally treated materials coupled with treatment of model compounds for sulfonic acids demonstrated that stability is related to the presence of activating and deactivating substituents on the aromatic system...
May 7, 2018: ChemSusChem
Kecheng Guan, Quan Liu, Yufan Ji, Mengchen Zhang, Yulin Wu, Jing Zhao, Gongping Liu, Wanqin Jin
Lignin-cation was rationally introduced into graphene oxide (GO) enabling stabilized nanostructure and active sites affording various interactions for subsequent modifications with polyelectrolyte and nano-spacers to precisely control the nanochannels of GO-based membranes. The resulting membranes exhibited excellent biofuel dehydration performance with water flux of 4000-6000 g m2 h-1 that transcends the state-of-the-art polymeric and GO-based membranes.
May 7, 2018: ChemSusChem
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