CHEMICAL ENGINEERING JOURNAL
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2013
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IF 3.473
Manhong Liu,Qiang Bai,Hailian Xiao,Yanyan Liu,Jun Zhao,William W. Yu
Colloidal platinum–ruthenium bimetallic nanoparticles with 2.3 nm were synthesized in solution and then immobilized on tin dioxide powder to make a supported nanocatalyst (Pt–Ru/SnO 2 ). The immobilized bimetallic nanoparticles had the same size and size distribution as the solution dispersed ones. Selective hydrogenation of o -chloronitrobenzene to o -chloroaniline was performed over the as-prepared Pt–Ru/SnO 2 nanocatalyst without using any solvent; 99.5% selectivity to o -chloroaniline at ∼100% conversion was achieved.
研究领域:
催化化学
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纳米材料
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有机合成
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绿色化学
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应用化学
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FOOD CHEMISTRY
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2023
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IF 8.8
Yalan Hu,Youyou Li,Yueru Shi,Yixin Kuang,Suxin Zhou,Yuan Peng,Yuefan Liu,Luyi Chen,Ningbo Zhou,Juan Zheng,Fang Zhu,Gangfeng Ouyang
Persistent organic pollutants (POPs) are widely distributed in the environment and are toxic, even at low concentrations. In this study, we first used hydrogen-bonded organic framework (HOF) to enrich POPs, based on solid phase microextraction (SPME). The HOF called PFC-1 (self-assembled by 1,3,6,8-tetra(4-carboxylphenyl)pyrene) has an ultra-high specific surface area, excellent thermochemical stability, and abundant functional groups, making it potential to be an excellent coating in SPME. And the as-prepared PFC-1 fiber have demonstrated outstanding enrichment abilities for nitroaromatic compounds (NACs) and POPs. Furthermore, the PFC-1 fiber was coupled with gas chromatography-mass spectrometry (GC–MS) to develop an ultrasensitive and practical analytical method with wide linearity (0.2–200 ng·L −1 ), low detection limits for organochlorine pesticides (OCPs) (0.070–0.082 ng·L −1 ) and polychlorinated biphenyls (PCBs) (0.030–0.084 ng·L −1 ), good repeatability (6.7–9.9%), and satisfactory reproducibility (4.1–8.2%). Trace concentrations of OCPs and PCBs in drinking water, tea beverage, and tea were also determined precisely with the proposed analytical method.
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FUEL PROCESSING TECHNOLOGY
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2023
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IF 7.5
Mengjiao Fan,Yuewen Shao,Kai Sun,Yuchen Jiang,Shu Zhang,Yi Wang,Song Hu,Jun Xiang,Xun Hu
Bio-oil as a carbon source can be used to prepare hybrid metal@carbon material while the polymerization of which generally prevents metals from exposure. In this study, melamine was used as a structural regulating agent for preparing Co/N/C catalyst via heating the mixture of cobalt nitrate, melamine and bio-oil for hydrogenation of o-chloronitrobenzene (o-CNB). The results showed that the Co species was encapsulated in the carbon structure from cross-polymerization of melamine and bio-oil at 600 °C. The further heating to 900 °C led to decomposition of melamine-derived substance, and meanwhile cobalt oxide was reduced and confined in the resulting carbon structure. The formed metallic Co catalyzed the growth of long carbon nanotube with cobalt on the tip, forming the Co/N/C catalyst of higher specific surface area (128.2 m 2 /g) and metallic Co dispersion (3.7%), rendering the superior activity for hydrogenation of o-CNB with the yield of o-chloroaniline up to 90.2%. The encapsulation or exposure of Co species was closely related to relative ratio of bio-oil and melamine in the catalyst precursors. Additionally, leaching of cobalt, due to dechlorination of o-CNB, was found to be an issue of Co/N/C catalyst but not for that of Ni/N/C catalyst.
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Jiasheng Wang,Ying Zhang,Xiaonan Xu,Ming Bao
Halogenated arylamines are important intermediates for the synthesis of dyes, pesticides, herbicides, and other chemicals. One important way to prepare halogenated arylamines is catalytic hydrogenation of halogenated nitroarenes. Ni-based catalysts have been used in the hydrogenation of halogenated nitroarenes but suffer from low activity and dehalogenation side reaction. In this paper, Ni–CeO2/SiO2 heterojunction catalyst with a “raisin-bun” structure was prepared by reverse microemulsion. A built-in electric field and more oxygen vacancies were formed due to electron transfer from Ni to CeO2 as a result of their work function difference. The built-in electric field leads to the heterolytic cleavage of H2, thereby improving the hydrogenation activity. Oxygen vacancies preferentially adsorb and activate nitro groups, inhibiting the dehalogenation side reaction. Through the cooperation of built-in electric field and oxygen vacancy, synchronous enhancement of the activity and selectivity is obtained successfully. This finding provides a new view for the design of non-noble metal-based catalysts with high activity and selectivity.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Ziqi Sun,Meiling Qi
This work presents the investigation of a novel CO 2 -based poly(ether-carbonate) copolymer, namely poly(propylene ether-carbonate)diol (PPCD), for gas chromatographic (GC) analyses. The PPCD column exhibited column efficiency of 4000 plates/m determined by naphthalene at 120 ℃ with the retention factor 6.23. Its separation performance was investigated by adopting a wide variety of analytes and isomers, including the isomer mixtures of alkanes, substituted benzene isomers with diverse groups, phenols and anilines, and the mixtures of organic solvents of high volatility, aliphatic amines and N-heterocycles. As a result, the PPCD column displayed distinctly higher resolving capability than the commercial columns described herein and achieved high column inertness towards acidic/basic analytes without involving any deactivation procedure. Additionally, it displayed excellent separation repeatability and reproducibility with the relative standard deviation (RSD) values less than 0.01% for within-day and in the range of 0.26% – 0.36% for between-day and 3.0% – 4.1% for between-column ( n = 4). Further, the PPCD column (30 m) was used to GC–MS analysis of the lemongrass essential oil and resolved more components well than the indicated commercial columns, evidencing its outstanding separation performance for analyses of complex samples. Up to date, the CO 2 -based poly(ether-carbonate) copolymers are not reported in the field of chromatography. This work demonstrates their promising future as a new type of selective and inert stationary phases for practical GC analyses.
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Molecular Catalysis
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2022
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IF 5.089
Jiarui Zhao,Lingzhe Fang,Junhong Fu,Jian Wang,Qike Jiang,Tao Li,Jiahui Huang
The performance of many supported metal catalysts is markedly enhanced by promoters. Here, we demonstrate the introduction of Mo into TiO 2 -supported IrMo catalysts greatly boosts the 3-vinylaniline (3-VA) selectivity of the hydrogenation of 3-nitrostyrene (3-NS). With the rise of Mo component in IrMo/TiO 2 catalysts, the Ir that activate H 2 are surrounded by more Mo species and become more oxidized, which prevents flat adsorption of 3-NS on Ir; meanwhile, Mo(V) species that are favorable for activation of nitro group of 3-NS increase, thus the synergistic effect affords excellent 3-VA selectivity. The optimal catalyst 1Ir9Mo/TiO 2 displays 99.8% selectivity of 3-VA at a 100% conversion. It also shows good recyclability and universality in selectively reducing unsaturated nitroarenes to corresponding anillines with exceptional selectivity.
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ACS Applied Nano Materials
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2022
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IF 6.14
Fan Yang,Hongbo Yu,Chunzheng Wu,Shiwei Wang,Tong Li,Hongfeng Yin
Supported Rh nanoparticles (NPs) exhibit excellent activity for the chemoselective hydrogenation of halonitrobenzenes (HNBs), but their selectivity to aromatic amines is not satisfactory due to the side reaction on the carbon–halogen bonds, and their recycling stability is limited due to the aggregation and the leaching of active component during the long-term usage. Herein, we design a yolk–shell-structured catalyst that consists of RhCu alloy cores and hollow/microporous carbon shells (HCS) to overcome these problems. The obtained RhCu@HCS catalyst with a Rh/Cu ratio of 1:1 showed good activity, selectivity, and stability in the hydrogenation of p-CNB (p-chloronitrobenzene) to produce p-CAN (p-chloroaniline) due to the synergistic effect between Rh and Cu. The protective carbon shells not only prevented the aggregation of metal NPs but also allowed the reactants to diffuse freely across the shells. Therefore, our research provides a general strategy to design highly efficient and stable hydrogenation catalysts.
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JOURNAL OF CATALYSIS
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2022
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IF 8.047
Lihua Zhu,Huan Zhang,Huaze Zhu,Huan Fu,Anna Kroner,Zhiqing Yang,Hengqiang Ye,Bing Hui Chen,Rafael Luque
Herein, we report a simple synthesis of PtNiCo trimetallic nanoparticles (NPs) loaded on carbon black (PtNiCo/C) via ambient-temperature chemical reduction and galvanic replacement reaction. The influence of thermal treatment temperature in 10 %H 2 /N 2 on PtNiCo NPs in PtNiCo/C-X nanostructures is revealed, where, X = 200 °C, 500 °C. XRD, XPS, TEM, HAADF-STEM, HRTEM, STEM-EDX elemental line-scanning (mapping), HS-LEIS, H 2 -TPR, atomic resolution aberration-corrected STEM (AC-STEM), XANES and EXAFS have been employed to characterize various nanostructures of PtNiCo NPs in PtNiCo/C-X. We established the relationship of nanostructure-reducing temperature thus catalytic behavior of PtNiCo/C-X: PtNiCo/C-200 ∼ Pt island (single atom and cluster)-on-NiCo alloy NP, PtNiCo/C-500 ∼ PtNiCo alloy NPs. PtNiCo/C-200 provides much improved catalytic activity and selectivity to target products ( NO 2 group hydrogenation) as compared to PtNiCo/C-500 for nitroarenes selective hydrogenation under mild reaction conditions (1.0 MPa-H 2 pressure, 18 °C or 40 °C-reaction temperature). That is considered to be closely correlated with the synergy effect of Pt islands and NiCo alloy nanoparticles in PtNiCo/C-200.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Liang Zhu,Xuecui Mei,Zhengchun Peng,Jiao Yang,Yingchun Li
Paper-based microfluidic analytical devices (μPADs) have recently attracted attention as a rapid test kit owing to their low cost and nonrequirement for external driving pump. However, low accuracy and poor anti-interference ability of μPADs under complex detection condition limit their practical applications. Here, we present a facile way to prepare a novel fluorescence sensor-array μPAD for multi-analyte discrimination based on molecular imprinting technology , and its sensing behavior was studied by using three nitrophenol (NP) isomers (2-, 3-, and 4-NP) as the testing models. Carbon quantum dots (CQDs) emitting blue light were grafted on glass-fiber paper, followed by in-situ modification of three types of molecularly imprinted polymers (MIPs) with 2-, 3-, and 4-NP as template. Each sensing unit on the array showed differential yet cross-reactive binding affinity to NP isomers, resulting in distinct fluorescence quenching efficiency. Thus, precise distinguishment of the three NPs was realized with the MIPs/CQDs/paper-based sensor array. Furthermore, the discrimination ability of the platform was evaluated in mixtures of the NP isomers. Practicability of this apparatus was validated by identification of blind samples and 100% accuracy was achieved. The μPAD has proven to be highly sensitive and accurate, which will serve as an ideal analytical tool in the fields of environment monitoring, disease prognosis, food safety and so on.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Zhijun Li,Mingyang Zhang,Xiuli Dong,Siqi Ji,Lili Zhang,Leipeng Leng,Honghong Li,J. Hugh Horton,Qian Xu,Junfa Zhu
The realization of efficient and fully controllable synthesis of single atom catalysts is an exciting frontier, yet still challenging in the modern catalysis field. Here we describe a straightforward high-temperature quenching approach to precisely construct isolated palladium atoms supported over cubic indium oxide, with individual palladium atoms coordinated with four neighboring oxygen atoms. This palladium catalyst achieves exceptional catalytic efficiency in the selective hydrogenation of nitrobenzene to aniline, with more than 99% chemoselectivity under almost 100% conversion. Moreover, it delivers excellent recyclability, anti-CO poisoning ability, storage stability, and substrate tolerance. DFT calculations further reveal that the high catalytic activity stems from the optimized electronic structure and the charge states of palladium atoms in the defect-containing indium oxide. Our findings provide an effective approach to engineering single atom catalysts at the atomic level and open the door to a wide variety of catalytic reactions .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Yebin Zhou,Ling Li,Yi Liu,Hongzheng Wang,Zhenlong Feng,Feng Feng,Qunfeng Zhang,Wucan Liu,Wenfeng Han,Chunshan Lu,Xiaonian Li
Most of the catalytic hydrogenation reactions take place under high temperature, high pressure, and high corrosion, which poses a challenge to the activity and stability of hydrogenation catalysts. Herein, an acid resistant and strawberry-like metal–carbon sphere (M/SCS) as a robust hydrogenation catalyst was synthesized by a one-step method. Self-assembled metal nanoparticles gather and are embedded on the surface of the carbon sphere prepared by the carbonization of phenolic resin. By means of the surrounding carbon layer, the acid resistant capability is orders of magnitude intensified compared to traditional commercial catalysts. Over 91.5% and 100% metals of Pd/SCS7 and Pt/SCS7 remain as the catalyst in hydrochloric acid (36–38 wt %), while less than 44.6% and 37.5% metals remain of commercial Pd/AC and Pt/AC. In addition, the sizes are controlled in the range of 11 to 18 nm for metal particles and 400 to 1600 nm for carbon spheres by adjusting the conditions of phenolic aldehyde condensation. N atoms anchored on the carbon spheres with high dispersion can improve electron density on metal particles. M/SCS exhibits both excellent stability and high catalytic performance in the hydrogenation reactions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Lixia Li,Qinkai Guo,Baohe Lv,Minxue Zheng,Wang Zhan,Yanhong Liu,Wanzhen Xu,Ruiwei Wang,Hongbo Zeng,Baodong Mao
The mixed-valent magnetite (Fe 3 O 4 ) played a critical role in H 2 O 2 -based Fenton-like system for the removal of chlorophenols, but high activity and cycle stability of the Fe 3 O 4 -based catalysts are still a huge challenge. Herein, a series of surface hydroxyl- and carboxyl-modified Ag 0 /Fe 3 O 4 nanocomposite catalysts were prepared and used to activate H 2 O 2 for degradation chlorophenols pollutants. Under the optimized condition, nearly 100% degradation ratio were achieved within 2–30 min for 2,4-dichlorophenol, 2,3-dichlorophenol, 3,4-dichlorophenol, 2,4,6-trichlorophenol, p-nitrophenol, and 98% degradation ratio for 2,5-dichlorophenol, 2,6-dichlorophenol and 3,5-dichlorophenol,. Moreover, wide pH applicability was obtained for the Ag 0 /Fe 3 O 4 -H 2 O 2 system, where 95% degradation ratio of 2,4-dichlorophenol was still obtained at pH 6.0. The excellent activity of Ag 0 /Fe 3 O 4 catalyst can be ascribed to the incorporation of Ag 0 nanoparticles that accelerated the Fe(III)/Fe(II) transformation with the assistance of surface hydroxyl and carboxyl groups. Detailed mechanism study indicated a pseudo-second-order kinetic model, where the oxidative degradation and reductive degradation pathways coexisted in the system. The surface-modified Ag 0 /Fe 3 O 4 -H 2 O 2 provide a practical catalyst system for the removal of phenol contaminants with high reaction rate, wide pH adaptability, and validity for a series of chlorophenols.
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