CATALYSIS TODAY
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2020
·
IF 5.825
Hong Du,Miao Jiang,Xiuyun Ma,Peifang Yan,Z. Conrad Zhang
The rapid consumption of fossil resources and the grim environmental situation encourage the application of renewable and clean energy resources. Conversion of biomass, which is a kind of renewable, CO 2 neutral as well as abundant reserves carbon containing resource, is significantly important. The production of fuels from biomass by means of gasification and Fischer-Tropsch synthesis is one of the most promising routes for industrial applications. The wax-free liquid fuels synthesis directly from H 2 -deficient syngas similar to bio-gas is highly advantageous for reducing investment and operating cost. Thus, the Mn-promoted meso-ZSM-5 supported cobalt catalyst was applied for the production of wax-free liquid fuels by catalytic H 2 -deficient syngas conversion in this study. The performance of the reaction was influenced obviously by Mn content. The cobalt dispersion increased with the addition of Mn, whereas the reduction degree decreased after Mn doping. Then, the balance between the dispersion and reduction degree led to the change in CO uptake followed a volcanic curve. The catalyst with moderate amount of Mn (1 wt%) had the suitable cobalt particle size and the maximum CO uptake. Thus, the highest CO conversion was obtained over Co-1Mn/meso-ZSM-5 catalyst thanks to its maximum exposed active sites. The appropriate amount of Mn addition also resulted in the decreasing of CH 4 selectivity. The highest space time yield of liquid fuels was acquired over the Co-1Mn/meso-ZSM-5 catalyst from H 2 -deficient syngas conversion under the moderate conditions.
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JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Qin Zhu,Jiaorong Yan,Qiguang Dai,Qingqing Wu,Yuanpu Cai,Jinyan Wu,Xingyi Wang,Wangcheng Zhan
A unique zeolite catalyst, Fe doped ZSM-5 microsphere assembled by uniform nanorod-like crystals with hierarchical pore structure, was successfully synthesized and applied for the adsorption and degradation of trace chlorobenzene (CB) in the presence of H 2 O 2 . The organic ferric salts as the precursors, ethylene glycol as a chelating/reducing agent and the dynamic two-stage temperature-varied hydrothermal technique, together made the synthesized hierarchical Fe-ZSM-5 nanorods assembled microspheres (FZ-CA-5EG) to be characterized by abundant highly dispersed and valency-controlled framework Fe 3+/2+ species. As a result of these features, the FZ-CA-5EG showed excellent ability of adsorption and degradation efficiency of CB, and enhanced durability due to negligible leaching of framework Fe species. Moreover, the hydroxyl radicals were determined as the main the reactive oxygen species of CB oxidation degradation, and a possible adsorption-oxidation degradation pathway was proposed.
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Materials Research Express
·
2019
·Vol. 6
·期 11
·115540
·
IF 1.449
Yong Liu,Qiong Luo,Hao Lu,Zhao Wang
The factors influencing the hydrothermal synthesis of ZSM-5 have been investigated in detail, such as silicon source, template, pH, reaction temperature, etc The type of template plays a key role. It is difficult to synthesize ZSM-5 without template or using inorganic template under our research conditions. However, the organic template of tetrapropylammonium bromide (TPABr) or n-butylamine (BTA) is beneficial to the synthesis of HZSM-5. The pH range of 10.79–11.14 is favorable for the synthesis of HZSM-5 zeolite. When temperature is greater than or equal to 160 °C, the synthesis of target zeolites is easy. However, if temperature is ≤140 °C, the synthesized product belongs to amorphous solid. Scanning electron microscopy (SEM) shows that the morphology of HZSM-5 crystal is hexagonal columnar. Fourier transform infrared (FTIR) analysis shows the synthesized product has a good ZSM-5 skeleton structure. The synthetic HZSM-5 zeolite has the BET specific surface area of about 387.326 m2 g−1. The adsorption capacities of the synthesized HZSM-5 for phenol, quinoline and indole can reach up to 43.54 mg g−1, 83.10 mg g−1 and 69.51 mg g−1, respectively.
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APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Yuxing Wang,Qingji Ying,Yaoyu Zhang,Yue Liu,Zhongbiao Wu
In this paper, the reaction behaviors of CH 3 CN catalytic combustion over CuCeO x -HZSM-5 catalysts prepared by the physical mixing and wet impregnation methods were investigated. The experimental results had revealed that the composite catalysts exhibited excellent degradation efficiency and high N 2 selectivity: the Cu-Ce oxides ensured the high activity, and the introduction of HZSM-5 limited the formation of NO x . The involved reaction mechanism was then studied by an in situ DRIFT analysis. It could be deduced that different reaction pathways would occur over CuCeO x and HZSM-5. The catalytic reaction over CuCeO x mainly proceeded via an oxidation pathway. The CN group could be converted to isocyanate species [NCO(a)] which would be further oxidized to NO x . Over HZSM-5, CH 3 CN was mainly hydrolyzed into ammonia. For the CuCeO x -HZSM-5 composite catalysts, the over-oxidation of NCO(a) and NH 3 was inhibited, and an internal selective catalytic reduction (SCR) reaction could occur, thereby greatly improving the N 2 selectivity.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Lifang Gao,Zhenbang Liu,Jinling Ma,Lijie Zhong,Zhongqian Song,Jianan Xu,Shiyu Gan,Dongxue Han,Li Niu
A key challenge for the conversion of 5-hydroxymethylfurfural (HMF) into value-added 2,5-furandicarboxylic acid (FDCA) is improving the sluggish kinetics of selective oxidation alcohol groups. Electrocatalysis has been proved to be a green and efficient strategy for heterogeneous synthetic chemistry. Herein, we report an electrocatalyst of NiSe@NiO x core-shell nanowires for efficiently upgrading HMF into FDCA. The NiSe@NiO x features conductive NiSe nanowires as a core and active NiO x as a shell, showing a smaller Tafel slope of 23 mV dec −1 accompanying with a near-quantitative yield of FDCA and 99% Faradaic efficiency (FE). X-ray photoelectron spectroscopy unveils the high valence of Ni species in the NiO x shell may be the active sites. Further integrated electrolyzer can produce FDCA and hydrogen simultaneously, showing a 100% FE even after six successive cycles, disclosing robust stability. All these results demonstrate NiSe@NiO x core-shell nanowires as a promising robust non-precious electrocatalyst for highly efficient biomass transformation.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2022
·
IF 8.025
Xinyi Xing,Xian Shi,Rui Hu,Ying Guan,Hui Gao,Siquan Xu
In this work, a series of (x)Hf-β zeolite catalysts were prepared by a simple wet impregnation method and used as bifunctional catalysts with Lewis and Brønsted acid sites for synthesizing 5-hydroxymethylfurfural (5-HMF) from cellulose in H 2 O (NaCl) -THF biphasic system. Characterization analysis of (x)Hf-β zeolite catalysts with ICP-OES, N 2 adsorption-desorption isotherm, XRD, FTIR , SEM, NH 3 -TPD and Py-FTIR indicated that the catalysts possessed favorable pore structure, appropriate acid strength and acidity. A superior 86.3 % cellulose conversion and 53.4 % 5-HMF yield could be obtained at 200 °C for 4 h by using (5 %)Hf-β zeolite as the catalyst. In addition, the catalytic system provided a favorable 5-HMF yield from other carbohydrates, including glucose (85.1 %), sucrose (80.6 %), starch (65.1 %), maltose (65.0 %), dextran (59.9 %), and Moso bamboo (21.9 %). Nevertheless, the recyclability of (5 %)Hf-β zeolite catalyst was unsatisfactory and the 5-HMF yield showed a downtrend from 53.4 % to 24.4 % after 5 cycles. The catalyst has promising potential for converting biomass materials into high-value platform compounds.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Bo Jiang,Jinzhe Li,Xinyi Chen,Lu Huang,Shan Luo,Ying Xing,Jing Deng,Shuang Song,Feilong Dong
Exploring an environmentally friendly and highly activation catalysts in the advanced oxidation processes (AOPs) basing on sulfate radicals (SO 4 − •) has shown great importance for the remediation of refractory contaminants. Herein, Fe 3 O 4 -wrapped ZSM-5 (Fe 3 O 4 @ZSM-5) was constructed as heterogeneous catalyst to remove ciprofloxacin (CIP) via peroxymonosulfate (PMS) activation, in which performance, kinetics and mechanism insight were investigated in depth. The removal efficiency of CIP reached 90 % by Fe 3 O 4 @ZSM-5 catalysts within 100 min reaction when the initial pH was 3.0. During the reaction, SO 4 − • and HO• were proved to be coexisted in reaction system and SO 4 − • played a critical role in CIP degradation according to the radical quenching experiments and electron paramagnetic resonance (EPR) measurements. Based on the catalyst characterization and Langmuir-Hinshelwood adsorption kinetics analysis, the synthesis of Fe 3 O 4 nanoparticles (NPs) and ZSM-5 accelerated the dispersion process and enhanced adsorption ability of Fe 3 O 4 NPs, which further promoted the local concentration of CIP and PMS on the surface. In addition, the cycling experiments and metal leaching tests demonstrated that Fe 3 O 4 @ZSM-5 catalysts were stable and could be conveniently reused by magnetic separation. In addition, the impacts of coexisting irons (Cl − , SO 4 2− , NO 3 − , HCO 3 − ) confirmed that Fe 3 O 4 @ZSM-5 was still effective in real water. This study demonstrated the promising prospect of Fe 3 O 4 @ZSM-5/PMS system in the application of degradation refractory organic pollutants .
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 9
·2813-2823
·
IF 2.936
Yang Jian,Li Xuemei,Zhang Jia,Tian Junying,Yao Xiaolan,Liu Hailong,Xia Chungu,Huang Zhiwei
Valuable 5-amino-1-pentanol (5-AP) was efficiently synthesized from biomass-derived dihydropyran over hydroxylapatite nanorod supported Ni catalysts (Ni-HAP), by coupling the in situ generation of 5-hydroxypentanal (5-HP, via the ring-opening tautomerization of 2-hydroxytetrahydropyran (2-HTHP)) and its subsequent reductive amination. The Ni-HAP catalyst with 10 wt% Ni loading exhibited the highest 5-AP yield than the other Ni-HAP catalysts with different Ni loadings and several commercial hydrogenation catalysts, including Ru/C, Pt/C and Pd/C, as well as Raney Ni. High Ni particles dispersion, high reducibility and acidic intensity were found to account for the superior catalytic performance of 10Ni-HAP. The effect of reaction parameters on the catalytic performance was investigated, and an excellent 5-AP yield of 92% was achieved under mild reaction conditions of 80 °C and 2 MPa H 2 . The stability of the Ni-HAP catalyst was studied using a continuous flow reactor, and the sintering of Ni nanoparticles was considered as the major reason for the decline in hydrogenation activity. Graphical Abstract The Ni-HAP catalyst exhibited high catalytic performance to synthesis 5-AP due to the high Ni particles dispersion, reducibility and acidic intensity.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Jiaxing Zhang,Ajuan Zhou,Limin Ren,Min Yang,Guangjin Hou,Anfeng Zhang,Chunshan Song,Xinwen Guo
A clear understanding of the acidity-activity relationship is an important prerequisite for designing functional materials in alkylation of benzene with methanol. Herein, a series of b -axis-oriented [Fe/Al]-MFI nanosheets with similar thickness but varied acidities were prepared by tuning Fe incorporation to systematically study the effect of acidity on their alkylation performance. Comprehensive physiochemical studies demonstrate that tetrahedral framework type Fe species are dominated. The incorporation of Fe significantly weakens the strong acid strength of zeolite thus endowing the samples with proper acidity, consequently showing a strong inhibition effect on the by-product ethylbenzene. Moreover, a long-term stable operation (>300 h) is further achieved over the [Fe]-S-1 nanosheets by optimizing the content of framework Fe. This work elucidates the important relationship between acidity and alkylation activity.
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Small
·
2023
·
IF 13.3
Baolong Zhang,Zijian Li,Yushang Zhou,Zhaohui Yang,Zhimin Xue,Tiancheng Mu
The Nickel-based catalysts have a good catalytic effect on the 5-hydroxymethylfurfural electrooxidation reaction (HMFOR), but limited by the conversion potential of Ni 2+ /Ni 3+ , 1.35 V versus RHE, the HMF electrooxidation potential of nickel-based catalysts is generally greater than 1.35 V versus RHE. Considering fluorine has the highest Pauling electronegativity and similar atomic radius of oxygen, the introduction of fluorine into the lattice of metal oxides might promote the adsorption of intermediate species, thus improving the catalytic performance. F is successfully doped into the lattice structure of NiCo 2 O 4 spinel oxide by the strategy of hydrothermal reaction and low-temperature fluorination. As is confirmed by in situ electrochemical impedance spectroscopy and Raman spectroscopy, the introduction of F weakens the interaction force of metal-oxygen covalent bonds of the asymmetric M T -O-M O backbone and improves the valence of Ni in tetrahedra structure, which makes it easier to be oxidized to higher valence active Ni 3+ under the action of electric field and promotes the adsorption of OH − , while the decrease of Co valence enhances the adsorption of HMF with the catalyst. Combining the above reasons, F-NiCo 2 O 4 shows superb electrocatalytic performance with a potential of only 1.297 V versus RHE at a current density of 20 mA cm −2 , which is lower than the most catalyst.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2023
·
IF 4.5
Jing Chen,Jiao Yang,Ying Chen,Jianbin Dong,Rong Deng,Lianqin Zhu
5-hydroxytryptamine (5-HT) is an important neurotransmitter that plays an important role in regulating mood, sleep, vomiting, cardiovascular function, libido and appetite. When its concentration level changes or exceeds a certain range, it can lead to a variety of diseases. In this study, bis (dithiophen-dibenzoic acid) nickel, [Ni(C 2 S 2 (C 6 H 4 COOH) 2 ) 2 ], was successfully synthesized and self-assembled with Zn(NO 3 ) 2 ·4H 2 O to form a oxidation–reduction active three-dimensional MOFs with a nickel-zinc bimetallic center. Multi-walled carbon nanotubes (MWCNTS) have good electrical conductivity, and the composite of 3D Ni Zn-MOF materials with unsaturated coordination and oxidation–reduction activity can improve the electrical conductivity and catalytic performance of the composite. The prepared Ni Zn-MOF/MWCNTs/GCE electrochemical sensor can be used for detecting 5-HT. Under the optimized conditions, the concentration range of 5-HT was 0.5–115 μM, and the detection limit (LOD) was 0.03 μM (S/N = 3). The recovery of 5-HT in urine samples was 99.94 % ∼ 102.02 %, which proved that the sensor has excellent practical application value.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yiyuan Tao,Shiying Fan,Xinyong Li,Jing Yang,Jingang Wang,Guohua Chen
Owing to the sluggish reaction kinetics, it is a promising yet challenging task to achieve the adequate electricity-driven catalytic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) in neutral conditions. Herein, we have prepared an elelctrocatalyst with interfacial coupling effect through in-situ growth of Cu phthalocyanine (CuPc) on Co 3 O 4 spinel (Co 3 O 4 /CuPc), which constructs an effective electrocatalytic system of HMF oxidation with overall oxidation value-added products yield and total Faraday efficiency up to 80% and 70%, respectively. The interfacial coupling effect between CuPc and Co 3 O 4 spinel improve catalytic activity by effectively boosting the interfacial charge transfer and reducing the formation energy of key *C 6 H 3 O 4 in the catalytic pathway according to the in situ Raman spectroscopy and DFT simulation. This work illustrates the significance of interfacial coupling effect for developing highly efficient electrocatalysts applied for neutral system of biomass oxidation.
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