NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 16
·7695-7703
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IF 3.925
Qi Wu,Changfeng Zhao,Qinzhong Wang,Jing Liu
This study proposes the efficient separation of Au(III)/Pd(II)/Pt(IV)/Rh(III) through the 2-mercaptobenzothiazole-functionalised ionic liquid ([C6mim][2MBT]) using a cloud point extraction system. Direct cloud point extraction of Au(III) (about 99.9%) was realised without involving any functionalised ionic liquids. A significant enhancement of the Pd(II) extraction performance was found by adding rationally constructed [C6mim][2MBT]. Consequently, a fairly high extraction percentage of about 99.4% was obtained. However, further advancement of the proposed cloud point extraction showed that it could not be applied for the preconcentration of Pt(IV) and Rh(III) without adding stannous chloride, which plays a critical role in the segregation and could be adjusted by changing the hydrochloric acid concentration. Under the optimised conditions, the Rh(III) extraction process shows a high yield percentage (ca. 83.0%), where the majority of Pt(IV) was enriched in the aqueous phase. In addition, the underlying possible extraction mechanism was investigated using UV-vis, FT-IR and TEM measurements, which indicated that TX-114 acted as a solvent for the extracted metals. The developed procedure reveals efficient direct Au(III)/Pd(II)/Pt(IV)/Rh(III) separation using [C6mim][2MBT] via cloud point extraction.
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Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 47
·18354-18365
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IF 8.262
Lin Han,Pengfei Wang,Hui Liu,Qiangqiang Tan,Jun Yang
Tailoring the internal structure and chemical composition of nanomaterials is an effective way to enhance their performance for a given application. Herein, we report a general wet-chemistry approach to produce copper (Cu)-based binary hollow nanostructures with well defined architectures and investigate their catalytic properties in electrochemical reactions. This strategy relies on the galvanic replacement between Cu seeds and noble metal precursors including ruthenium (Ru), rhodium (Rh), palladium (Pd), osmium (Os), iridium (Ir), and platinum (Pt) in oleylamine at an appropriate temperature, which is essential to balance the reduction kinetics of the noble metal precursors by oleylamine during their galvanic replacement with Cu seed particles. Typically, the bimetallic CuPt hollow nanostructures with polyhedral morphologies exhibit enhanced catalytic properties for the oxygen reduction reaction (ORR), while their spherical counterparts obtained at a relatively low temperature show high activity for the methanol oxidation reaction (MOR). In particular, we will also demonstrate a unique application of the CuRu hollow nanostructures in supercapacitors after converting them into binary metal oxides at elevated temperatures in air.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Mei Ming,Yanlin Ren,Min Hu,Yun Zhang,Ting Sun,Yuling Ma,Xiaojing Li,Weidong Jiang,Daojiang Gao,Jian Bi,Guangyin Fan
Exploring MXenes as supports for synthesis of highly efficient catalysts are extremely important for hydrodechlorination of chlorophenols because of the acute toxicity and strong potential bioaccumulation of chlorophenols. We reported a facile strategy to synthesize Rh nanoparticles deposited on 2D alk-Ti 3 C 2 X 2 (X = O, F) (alk-Ti 3 C 2 X 2 for short) MXene, which was prepared through the removal of the Al layers of Ti 3 AlC 2 and post-treatment by alkalization. Modifying the Ti 3 C 2 X 2 support by alkalization triggered the substitution of surface fluorine groups with surface oxygen species. The changes in the surface chemistry of alk-Ti 3 C 2 X 2 effectively prevented particle aggregation to form well-dispersed Rh nanoparticles in small sizes with relative high metal dispersion, thereafter improving the hydrogen uptake capacity of the catalyst. Consequently, the Rh/alk-Ti 3 C 2 X 2 catalyst significantly enhanced the catalytic performance for the HDC reaction, which could be assigned to the large number of active components from small Rh nanoparticles. This strategy provides a basis for investigating the use of MXenes as supports to synthesize well-defined metal nanoparticles in 2D layered structures for potential applications.
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RSC Advances
·
2013
·Vol. 4
·期 2
·794-804
·
IF 2.562
Han Zhu,Ming Zhang,ShengYing Cai,YingTing Cai,Pan Wang,ShiYong Bao,MeiLing Zou,MingLiang Du
A facile approach for the synthesis of uniform, small size and well-dispersed rhodium nanoparticles (RhNPs) on cross-linked polyvinyl alcohol–polyethyleneimine (PVA–PEI) nanofibers has been demonstrated. Various methods were firstly employed to cross-link PVA nanofibers and the cross-linked PVA–PEI nanofibers exhibited good water stability and porous structures after immersing in water for 72 h. Because of the strong chelate effects among the amine groups, hydroxyl groups and Rh3+ ions, uniform RhNPs with an average diameter of about 2.5 ± 0.2 nm can evenly and densely grow throughout the PVA–PEI nanofibers via an in situ reduction. Meanwhile, the better dispersion and smaller size of the RhNPs grown on the nanofibers in comparison with the pre-synthesized RhNPs directly deposited on the nanofibers exhibit the advantages of in situ reduction for size and dispersion control. The successful fabrication of the RhNPs/(PVA–PEI) nanofibers with various densities of well-dispersed RhNPs demonstrates that the strong chelate effects and stabilization of the PVA–PEI nanofibers also play an essential role in the size and dispersion control of RhNPs. The crystal structures, chemical bonding and interactions of the prepared nanofibers were verified using XPS and FTIR spectra and XRD patterns. These novel nanomaterials were fabricated as non-enzymatic electrochemical sensors and exhibit highly electrocatalytic activity towards H2O2.
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TETRAHEDRON-ASYMMETRY
·
2014
·
IF 2.165
Rui-Jie Chen,Gao-Wei Zheng,Yan Ni,Bu-Bing Zeng,Jian-He Xu
A new NADH-dependent carbonyl reductase Rh CR capable of efficiently reducing the ε-ketoester ethyl 8-chloro-6-oxooctanoate (ECOO) to give ethyl ( S )-8-chloro-6-hydroxyoctanoate [( S )-ECHO], an important chiral precursor for the synthesis of ( R )-α-lipoic acid, was identified from Rhodococcus sp. ECU1014. Using recombinant Escherichia coli cells expressing Rh CR and glucose dehydrogenase used for the regeneration of cofactor, 440 g L −1 (2 M) of ECOO were stoichiometrically converted to ( S )-ECHO in a space–time yield of 1580 g L −1 d −1 without the external addition of any expensive cofactor.
研究领域:
生物催化
·
酶工程
·
合成化学
·
生物技术
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高影响因子
Journal of Cleaner Production
·
2025
·
IF 10
Tao Jiang,Ming Cheng,Yujiao Wang,Shaoqiang Guo,Wentao Zhou,Yafei Wang
The selective removal of neutron-absorbing fission products from spent nuclear fuel is critical for enhancing neutron economy and enabling efficient recycling. In this work, we present a novel two-step dry reprocessing strategy that integrates NH 3 /HCl gas mixture treatment with liquid Sn extraction to achieve phase-selective separation of Sm, Nd, Ru, Rh, and Pd from simulated U 3 O 8 -based spent fuel. Thermodynamic analysis and experimental validation reveal that decomposition of NH 4 Cl at elevated temperatures serves as the generator of NH 3 /HCl gas mixture capable of selectively chlorinating Sm 2 O 3 and Nd 2 O 3 into soluble chlorides while reducing U 3 O 8 to UO 2 and converting RuO 2 , Rh 2 O 3 , and PdO to their metallic states (Ru, Rh, Pd). Subsequent dissolution tests in LiCl-KCl confirm that Sm and Nd are almost completely removed, with chlorination efficiencies of nearly 100%, while uranium loss can be minimized by controlling direct NH 4 Cl contact. The coupled liquid Sn extraction at 1173 K enabled the recoveries of metallic Rh, Rh, and Pd with a promising extraction efficiency. This integrated approach significantly simplifies the partitioning of key neutron poisons (Sm, Nd, Ru, Rh, Pd) compared to conventional aqueous or pyrochemical routes, reduces secondary waste, and preserves uranium in its UO 2 form.
研究领域:
核化学
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放射化学
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核燃料循环
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材料化学
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湿法冶金
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热力学分析
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yuzhe Cao,Xunkai Zhu,Zejuan Ni,Bo Ge,Wei Li,Guina Ren,Xiao Miao,Xin Shao,Cancan Liu
Freshwater has become a rare resource on account of population increase and environmental pollution. At present, most the solar-driven interfacial evaporators used for water polluted by organic solvents and dyes have an outstanding nature of clean water production due to their special design. However, its downside is that contaminants remaining in the residual polluted water cannot be removed. Herein, a device applied to water polluted by organic solvents and dyes is formed by a hydrogel-based interfacial evaporator (PVA hydrogel/CNTs) and non-wetting fabric. The photodegradation efficiency of the non-wetting fabric is 95.7% for Rh B dye after five cycles. Meanwhile, the organic solvents including toluene, cyclohexane and so on are cleared through the non-wetting fabric. Importantly, the device presents a clean water production rate of 1.73 kg·m −2 ·h −1 under 1 sun illumination and it has a freshwater produce rate of 1.63 kg·m −2 ·h −1 after 6 h of desalination experiments. Furthermore, the device displays the performance of salt resistance in a 3 h NaCl dissolution experiment. A new strategy is provided for interfacial water evaporation technology used for water dyed by organic solvents and dyes purification and has a great application potential.
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ELECTROPHORESIS
·
2021
·
IF 3.535
Yanru Liu,Xia Wang,Jia Yu,Xingjie Guo
Enantiomeric separation of six antihistamine agents was first systematically investigated on a cellulose-based chiral stationary phase (CSP), that is, cellulose tris-(3,5-dimethyl phenyl carbamate) (Chiralcel OD-RH), under the reversed-phase mode. Orphenadrine, meclizine, terfenadine, dioxopromethazine, and carbinoxamine enantiomers were completely separated under the optimized mobile phase conditions with resolutions of 5.02, 1.93, 1.68, 1.67, and 1.54, respectively. Mequitazine was partially separated with a resolution of 0.77. The influences of type and concentration of buffer salt, the pH of buffer solution, and the type and ratio of organic modifier on the chiral separation were evaluated and optimized. For a better insight into the enantiorecognition mechanisms, molecular docking was carried out via the Autodock software. The lowest binding energy and the optimal conformations of the analytes/CSP complexes were supplied, and the mechanisms of chiral recognition were determined. According to the results, the key interactions for the chiral recognition of these six analytes on CDMPC were π–π interactions, hydrophobic interactions, hydrogen bond interactions, and some special interactions.
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高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 11
·5595-5600
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IF 11.301
Kai Deng,Tianlun Ren,You Xu,Songliang Liu,Zechuan Dai,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Although recent studies on the hydrogen evolution reaction (HER) have achieved great progress, it remains a great challenge to fabricate highly efficient pH-universal HER electrocatalysts. In this work, we report the facile synthesis of a new class of Rh-based spongy aerogels co-incorporated with transition metal M (M = Co, Ni, and Fe) and boron atoms through a simple and versatile one-pot wet-chemical strategy. Benefiting from the synergetic effect of 3D network-shaped spongy architectures and the electronic interaction between various elements, the optimized RhCoB aerogels exhibit excellent catalytic activity, stability and durability toward the HER in a wide pH range. The successful synthesis of RhMB aerogels will provide guidelines for designing and synthesizing an unprecedented class of transition metal and/or non-metal atom doped metallic materials toward potential catalysis and energy applications.
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Small Methods
·
2023
·
IF 12.4
Siyuan Lin,Zhenxing Fang,Jiao Ma,De'en Guo,Xiaohan Yu,Haipeng Xie,Mei Fang,Dou Zhang,Kechao Zhou,Yongli Gao,Conghua Zhou
“Perovskite/carbon” interface is a bottle-neck for hole-conductor-free, carbon-electrode basing perovskite solar cells due to the energy mismatch and concentrated defects. In this article, in-situ healing strategy is proposed by doping octylammonium iodide into carbon paste that used to prepare carbon-electrode on perovskite layer. This strategy is found to strengthen interfacial contact and reduce interfacial defects on one hand, and slightly elevate the work function of the carbon-electrode on other hand. Due to this effect, charge extraction is accelerated, while recombination is obviously reduced. Accordingly, power conversion efficiency of the hole-conductor-free, planar perovskite solar cells is upgraded by ≈50%, or from 11.65 (± 1.59) % to 17.97 (± 0.32) % (AM1.5G, 100 mW cm −2 ). The optimized device shows efficiency of 19.42% and open-circuit voltage of 1.11 V. Meanwhile, moisture-stability is tested by keeping the unsealed devices in closed chamber with relative humidity of 85%. The “in-situ healing” strategy helps to obtain T 80 time of >450 h for the carbon-electrode basing devices, which is four times of the reference ones. Thus, a kind of “internal encapsulation effect” has also been reached. The “in situ healing” strategy facilitates the fabrication of efficient and stable hole-conductor-free devices basing on carbon-electrode.
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高影响因子
GREEN CHEMISTRY
·
2017
·Vol. 19
·期 14
·3400-3407
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IF 9.125
Junjie Zhou,Yunong Li,Hong-bin Sun,Zhike Tang,Li Qi,Lei Liu,Yongjian Ai,Shuang Li,Zixing Shao,Qionglin Liang
A core–shell structured nanocatalyst (Fe3O4@SiO2-NH2-RhNPs@mSiO2) that is encapsulated with porous silica has been designed and prepared for catalyzing the transfer hydrogenation of nitro compounds into corresponding amines. Rh nanoparticles serve as the activity center, and the porous silica shell plays an important role in the “slow-release” of the hydrogen source hydrazine. This reaction can be carried out smoothly in the green solvent water, and the atom economy can be improved by decreasing the amount of hydrazine hydrate used to a stoichiometric 1.5 equivalent of the substrate. Significantly, high catalytic efficiency is obtained and the turnover frequency (TOF) can be up to 4373 h−1 in the reduction of p-nitrophenol (4-NP). A kinetics study shows that the order of reaction is ∼0.5 towards 4-NP, and the apparent active energy Ea is 58.18 kJ mol−1, which also gives evidence of the high catalytic efficiency. Additionally, the excellent stability of the catalyst has been verified after 15 cycles without any loss of catalytic activity, and it is easily recovered by a magnet after reaction due to the Fe3O4 nucleus.
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Nanoscale Advances
·
2020
·Vol. 2
·期 4
·1685-1693
·
IF 0
Wenxiu Luo,Xue Zhao,Wei Cheng,Yun Zhang,Yi Wang,Guangyin Fan
Metal nanoparticles (NPs) deposited on nitrogen (N)- and/or phosphorus (P)-doped porous carbon have been investigated as efficient catalysts for hydrolysis of ammonia borane (AB). However, the one-pot synthesis of N,P co-doped porous carbon using low-cost and readily available sources is still a tremendous challenge. Herein, a novel one-pot methodology is developed to fabricate N and P co-doped porous carbon (ATP-C) using non-precious and easily available adenosine triphosphate (ATP). The process of N and P doping does not need additional N or P sources in the material. Moreover, the entire process did not require chemical activation agents, making it more practical for large-scale applications. The resulting ATP-C supported Rh NPs (Rh/ATP-C) exhibit excellent performance for the catalytic hydrolysis of ammonia borane toward hydrogen generation, with a total turnover frequency (TOF) value of 566 mol H2 min−1 (mol Rh)−1 and activation energy (Ea) of 26.3 kJ mol−1. The catalytic system has shown an outstanding catalytic cycle life during the recycling tests. This work provides a novel method for the production of high performance carbon material supported metal NP catalysts for practical dehydrogenation applications.
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