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Frontiers of Chemical Science and Engineering · 2017 ·Vol. 11 ·期 4 ·564-574 · IF 1.712

The effect of doping and steam treatment on the catalytic activities of nano-scale H-ZSM-5 in the methanol to gasoline reaction

Song Baodong,Li Yongqiang,Cao Gang,Sun Zhenhai,Han Xu

In the transformation of methanol to gasoline (MTG), the selectivity to gasoline and the aromatic content in the produced gasoline are important factors. The catalytic activities of steam-treated and non-steam-treated nano-scale H-ZSM-5 (NHZ5) catalysts impregnated with Ag(I), Zn(II) or P(V) have been investigated in a continuous flow fixed bed reactor. The NH 3 -TPD results showed that after impregnation, the Ag/NHZ5, Zn/NHZ5 and P/NHZ5 catalysts contained comparatively more strong, medium-strong and weak acid sites, respectively. Treatment with steam decreased the number of acid sites in all the catalysts, but the pore volumes in the catalysts were larger which improved carbon deposition resistance resulting in prolonged lifetimes. After 6 h of MTG reaction, the selectivity to gasoline for the steam-treated catalysts, \(Ag_{H_2 O} /NHZ5\) , \(Zn_{H_2 O} /NHZ5\) and \(P_{H_2 O} /NHZ5\) were 70.5, 68.4 and 68.7 wt-%, respectively, whereas their respective aromatic contents in the produced gasoline were 61.9, 55.4 and 39.0 wt-%. Thus \(P_{H_2 O} /NHZ5\) is the most promising catalyst for MTG applications which can meet the China IV gasoline standard that the amount of aromatics in gasoline should be less than 48 wt-%.

研究领域: 催化化学 · 能源化工 · 材料科学 · 表面科学 · 石油炼制
✓ 已验证 DOI 高影响因子
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Chemical Engineering Journal Advances · 2020 · IF 0

In/H-Beta modified by Co3O4 and its superior performance in the presence of H2O and SO2 for selective catalytic reduction of NOx with CH4

Jiuhu Zhao,Zhengzhong Wen,Rongshu Zhu,Zhi Li,Ran Ding,Yongji Zhu,Tingkun Gu,Rong Yang,Zhenye Zhu

In this paper, In-metal oxide/H-Beta catalysts were synthesized by ion exchange method and In-Co 3 O 4 /H-Beta exhibited the highest catalytic activity for the selective catalytic reduction of NO x with CH 4 in presence of H 2 O and SO 2 . Thus, the synthesis conditions of In-Co 3 O 4 /H-Beta were optimized. The results showed that In-Co 3 O 4 /H-Beta exhibited excellent catalytic performance and high CH 4 selectively when the synthesis was carried out by ion exchange method, the ratio of Si and Al in H-Beta was 25, the ratio of Co 3 O 4 and H-Beta was 5:40, the concentration of ion exchange liquid was 0.033 M and calcination temperature was 500 °C. The NO x removal efficiency was about 87.6 % and N 2 selectivity could reach 96.3% in the presence of H 2 O and SO 2 . Through a series of characterizations, it was concluded that In-Co 3 O 4 /H-Beta owned stable catalyst structure, abundant Brønsted acid sites and the highest ratio of InO + /In 2 O 3 under the optimal synthesis conditions. In addition, the doped of Co 3 O 4 could inhibit the adsorption of sulfate species on the surface of In/H-Beta catalyst, leading to the excellent H 2 O and SO 2 resistance property.

研究领域: 环境科学 · 催化化学
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JOURNAL OF ORGANIC CHEMISTRY · 2024 · IF 3.3

Minisci-Type Dehydrogenative Coupling of N-Heteroaromatic Rings with Inert C(sp3)–H Enabled by a Visible-Light-Catalyzed Intermolecular Hydrogen Atom Transfer Process

Jun-Feng Yang,Yun-Fei Liu,Lin-Lin Wei,Kai-Kai Qiao,Yan-Qiu Zhao,Lei Shi

The Minisci-type dehydrogenative coupling of N-heteroaromatic rings with inert C–H or Si–H partners via visible-light-catalyzed hydrogen atom transfer has been reported. This methodology allows the coupling reactions to be carried out in water as a solvent under air atmospheric conditions with visible-light illumination. A wide range of inert C–H and Si–H partners could be directly coupled with various N-aromatic heterocycles to deliver products in good to excellent yields.

研究领域: 有机化学 · 光化学
✓ 已验证 DOI PubMed 高影响因子
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RARE METALS · 2023 ·Vol. 43 ·期 3 ·1153-1166 · IF 8.8

Layered niobium carbide enabling excellent kinetics and cycling stability of Li-Mg-B-H hydrogen storage material

Lu Li-Wen,Luo Hui,Li Guang-Xu,Li Yun,Wang Xin-Hua,Huang Cun-Ke,Lan Zhi-Qiang,Zhou Wen-Zheng,Guo Jin,Ismail Mohammad,Liu Hai-Zhen

The Li-Mg-B-H composite (2LiBH 4  + MgH 2 ) has a high capacity of 11.4 wt% as a hydrogen storage material. However, the slow kinetics and poor cycling stability severely restrict its practical applications. In this work, a layered Nb 2 C MXene was first synthesized and then introduced to tailor the kinetics and cycling stability of the Li-Mg-B-H composite. The milled 2LiH + MgB 2 composites were initially hydrogenated to obtain the 2LiBH 4  + MgH 2 composites. The 2LiBH 4  + MgH 2  + 5 wt% Nb 2 C can release 9.0 wt% H 2 in 30 min at 400 °C, while it is only 2.7 wt% for the undoped 2LiBH 4  + MgH 2 . The dehydrogenation activation energies of MgH 2 and LiBH 4 are 123 and 154 kJ·mol −1 respectively for the 5 wt% Nb 2 C-doped composite, lower than the undoped composite (164 and 165 kJ·mol −1 ). The 2LiBH 4  + MgH 2  + 5 wt% Nb 2 C possesses excellent cycling stability, with the reversible capacity only slightly reduced from 9.4 wt% for the 1st cycle to 9.3 wt% for the 20th cycle. Nb 2 C keeps stable in the composite and acts as an efficient catalyst for the Li-Mg-B-H composite. It is believed that both the layered structure and the active Nb element contribute to the enhanced hydrogen storage performances of the Li-Mg-B-H composite. This work confirms that the Nb 2 C MXene with layered structure has a significant enhancing impact on the Li-Mg-B-H hydrogen storage materials, which is different from the bulk NbC. Graphical abstract

研究领域: 材料科学 · 能源化学 · 纳米催化 · 储氢技术 · 固体化学
✓ 已验证 DOI 高影响因子
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DALTON TRANSACTIONS · 2020 ·Vol. 50 ·期 3 ·1060-1068 · IF 4.174

Regioselective B(3)–H bond activation based on an o-carboranyl dithiocarboxylate ligand and its derivatives

Run-Ze Yuan,Peng-Fei Cui,Shu-Ting Guo,Guo-Xin Jin

Herein, we describe the synthesis of tetraphenylphosphonium o-carboranyl dithiocarboxylate (Ligand 1) and methyldithiocarboxyl-o-carborane (Ligand 2). The complexes [Cp*M(o-C2B10H11CS2)Cl] (M = Ir (3); Rh (4)) and [Cp*M(o-C2B10H11CS2)2] (M = Ir (5); Rh (6)) have been synthesized based on Ligand 1. The selective B–H bond activation of Ligand 2 has also been explored, leading to the synthesis of the B–H activated complex [Cp*Ir(o-C2B10H10CS2CH3)Cl] (7) and four of its substituted derivatives (8, 9, 10 and 11). All of these compounds have been characterised through single-crystal X-ray diffraction, NMR, IR spectroscopy and elemental analysis.

研究领域: 无机化学 · 配位化学
✓ 已验证 DOI 高影响因子
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ADVANCED SYNTHESIS & CATALYSIS · 2017 ·Vol. 359 ·期 13 ·2215-2221 · IF 5.646

One-Pot Three-Component Synthesis of Alkylthio-/Arylthio- Substituted Imidazo[1,2-a]pyridine Derivatives via C(sp2)–H Functionalization

Wenhui Zhu,Yingcai Ding,Zhaogang Bian,Ping Xie,Baojun Xu,Qiujie Tang,Wei Wu,Aihua Zhou

Sulfenylation is an important transformation to generate C−S bonds in organic synthesis. Here, two three-component synthetic protocols have been developed by using imidazo[1,2- a ]pyridine, inorganic, odorless S 8 and alcohols or arylboronic acids as reactants to make alkylthio-/arylthio-substituted imidazo[1,2- a ]pyridine derivatives via C( sp 2 )–H functionalization. The reactions proceeded with high efficiency and broad functional group tolerance, affording the products regioselectively and in good yields.

研究领域: 有机化学 · 药物化学
✓ 已验证 DOI 高影响因子
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Catalysts · 2020 ·Vol. 10 ·期 6 ·695 · IF 3.52

Facile Formation of Anatase Nanoparticles on H-Titanate Nanotubes at Low Temperature for Efficient Visible Light-Driven Degradation of Organic Pollutants

Weiwei Fu,Zhiqiang Shi,Helong Bai,Jinyu Dai,Zhiming Lu,Feifei Lei,Deguang Zhang,Lun Zhao,Zongtao Zhang

Anatase nanoparticles (5–10 nm) generated on H-titanate nanotube surface (H-titanate/anatase) were prepared by an ingenious and simple method. H-titanate tubes were prepared by a hydrothermal reaction of Ti powder in concentrated NaOH solution and an ion exchange process with HNO3solution. After that, at a relatively low drying temperature (100 °C), a small quantity of anatase nanoparticles were in-situ formed on the H-titanate tubes surface by a surface dehydration reaction. In-situ transformation can form a strong interface coupling between H-titanate and anatase, which is conducive to accelerating charge transfer and improving its photocatalytic activity. In addition, the smaller average crystal size, the large specific surface areas (BET), the nanotubed and layered structure and the synergistic effect of dual phases would be beneficial to improving the photocatalytic efficiency.

研究领域: 材料科学 · 环境科学
✓ 已验证 DOI 高影响因子
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Sustainable Energy & Fuels · 2021 ·Vol. 6 ·期 2 ·440-448 · IF 6.367

Constructing multi-functional composite separator of PVDF-HFP/h-BN supported Co-CNF membrane for lithium–sulfur batteries

Xin Liang,Lulu Wang,Yang Wang,Yongchao Liu,Yi Sun,Hongfa Xiang

The functional design of separators has been proved to be one of the most efficient methods to improve the electrochemical performance of lithium–sulfur batteries. In this work, a multifunctional separator with gradual changes to four aspects was constructed by integrating a PVDF-HFP/h-BN membrane with a Co-doped carbon nanofiber. The architecture has four gradations, which offers multifold advantages. First, in terms of density, there is a transition from loose to dense, which results in a higher electrolyte uptake rate, reduces the amount of free electrolyte and further suppresses the shuttle effect. Additionally, in terms of composition, a transition from inorganic to organic is designed, which allows the inorganic and organic components to bind closely and reduces the interfacial resistance. Meanwhile, there is a transition from high electronic conductivity to insulation. The change in electronic conductivity leads to effective conversion of the polysulfide. Finally, in terms of ionic conductivity, there is a transition from low to high, which gives the separator better ability to conduct lithium ions. As a consequence, a battery with the as-constructed multifunctional separator performs with good capacity stability, which demonstrates a new concept for high-performance lithium–sulfur battery design.

研究领域: 材料科学 · 储能技术 · 电池技术
✓ 已验证 DOI 高影响因子
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Molecular Catalysis · 2019 · IF 2.938

Ru/H-beta as an efficient catalyst for the conversion of furfural into 3-acetyl-1-propanol (3-AP) toward one-pot transformation of xylan to 3-AP

Qiaoyun Liu,Fei Liu,Yaru Zhang,Yang Su,Aiqin Wang,Tao Zhang

A highly active and robust catalyst composed of Ru nanoparticles highly dispersed on zeolite H-beta was developed for transforming furfural into 3-acetyl-1-propanol (3-AP) in good yield (81%)under mild conditions (80 °C, 1 MPa H 2 ). Both the support nature and the preparation methods had significant impacts on the dispersion of Ru, eventually on the yield of 3-AP. Ion-exchange method proved best for obtaining the highly active and selective catalyst for this reaction. Moreover, the catalyst can be regenerated easily by calcination and reduction. This catalyst was further explored for the one-pot conversion of xylose and xylan to 3-AP with a yield of 46% and 31%, respectively, thus opening a new feasible pathway from biomass to valuable fine chemicals.

研究领域: 催化化学 · 生物质转化 · 绿色化学
✓ 已验证 DOI 高影响因子
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BMC Chemistry · 2019 ·Vol. 13 ·期 1 ·1-15 · IF 0

Highly selective cleavage C–O ether bond of lignin model compounds over Ni/CaO–H-ZSM-5 in ethanol

Guo J.,Ma Yu L.,Yu Jia Y.,Gao Yu J.,Ma Ning X.,Wu Xiao Y.

Herein, 2-(2-methoxyphenoxy)-1-phenylethanol (β- O -4), 2-methoxyphenyl anisole (α- O -4) and 4-phenoxyphenol (4- O -5) were selected as typical lignin model compounds. Given the effectiveness of traditional acid–base catalysts for lignin depolymerisation, a novel Ni/CaO–H-ZSM-5(60) catalyst was prepared to investigate the difficulty level of C–O bond of three model compounds cleavage in ethanol. It was observed that Ni/CaO–H-ZSM-5(60) had prominent performance on the C–O bond cleavage at very mild conditions (140 °C, 1 MPa H 2 ). Among them, the C–O bond of α- O -4 and β- O -4 could be completely cleaved within 60 min. Although the C–O bond of 4- O -5 had high bond energy, 41.2% of conversion was occurred in 60 min. The introduction of CaO could regulate the acidity of H-ZSM-5 to enhance the ability to break C–O bonds. Moreover, the possible pathways of C–O ether bonds in three lignin model compounds cleavage were proposed in order to selectively obtain target products from the raw lignin degradation.

研究领域: 化学工程 · 催化科学
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Journal of Energy Chemistry · 2023 · IF 13.1

Sn-doped BiOCl nanosheet with synergistic H+/Zn2+ co-insertion for “rocking chair” zinc-ion battery

Yuzhu Qian,Hongrui Wang,Xinni Li,Ting Song,Yong Pei,Li Liu,Bei Long,Xiongwei Wu,Xianyou Wang

The development of insertion-type anodes is the key to designing “rocking chair” zinc-ion batteries. However, there is rare report on high mass loading anode with high performances. Here, {001}-oriented BiOCl nanosheets with Sn doping are proposed as a promising insertion-type anode. The designs of cross-linked CNTs conductive network, {001}-oriented nanosheet , and Sn doping significantly enhance ion/electron transport, proved via experimental tests and theoretical calculations (density of states and diffusion barrier). The H + /Zn 2+ synergistic co-insertion mechanism is proved via ex situ XRD, Raman, XPS, and SEM tests. Accordingly, this optimized electrode delivers a high reversible capacity of 194 mA h g −1 at 0.1 A g −1 with a voltage of ≈0.37 V and an impressive cyclability with 128 mA h g −1 over 2500 cycles at 1 A g −1 . It also shows satisfactory performances at an ultrahigh mass loading of 10 mg cm −2 . Moreover, the Sn-BiOCl//MnO 2 full cell displays a reversible capacity of 85 mA h g −1 at 0.2 A g −1 during cyclic test.

研究领域: 材料科学 · 电化学 · 能源存储
✓ 已验证 DOI 高影响因子
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APPLIED CATALYSIS A-GENERAL · 2021 · IF 5.706

Microporous cobaltporphyrin covalent polymer mediated Co3O4@PNC nanocomposites for efficient catalytic C-H bond activation

Mingyang Tan,Liang Zhu,Hao Liu,Yajun Fu,Shuang-Feng Yin,Weijun Yang

A Cobalt porphyrin conjugated porous polymer (Co/PCP) was obtained by hybrid polymerization of a mixture of Co(II)(5,10,15,20-tetrakis(4-bromophenyl)-21H,23H-porphyrin) (CoTBPP) and 5,10,15,20-tetrakis(4-bromophenyl)-21H,23H-porphyrin (TBPP) (3:7 M ratio) with the coupling reagent of p-phenyldiboric acid. This Co/PCP was carbonized at 400 °C and the obtained catalyst (denoted as Co 3 O 4 @PNC-400) was composed of Co 3 O 4 nanoclusters wrapped in the nitrogen-carbon materials. This catalyst has an extremely high catalytic activity for the aerobic oxidation of C–H bonds. It can efficiently catalyze the oxidation of the C–H bonds in toluene and cyclohexane with high conversion and high selectivity of (alcohol + aldehyde), (alcohol + ketone) compounds, respectively. When heat-treated at 400 °C, the porous framework structure of the porphyrin polymer was partially retained, and the highly active Co 3 O 4 nanoclusters were generated in situ. The reaction of C N to C N and connection with the Co 3 O 4 nanoclusters also occurred. Co 3 O 4 @PNC-400 has obvious synergistic catalytic effect between Co 3 O 4 and nitrogen-carbon framework during the catalytic reaction. The defective structure caused by the migration of cobalt also greatly improved the catalytic activity. Co/PCPs with different cobalt contents were also synthesized and heat treated at different temperature. These catalysts were a new type of efficient C–H oxidation catalysts with excellent potential application value.

研究领域: 材料科学 · 催化 · 化学工程 · 有机化学
✓ 已验证 DOI 高影响因子
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