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Synthesis, physicochemical characterizations and catalytic performance of Pd/carbon-zeolite and Pd/carbon-CeO

Zeinab JAMALZADEH, Mohammad HAGHIGHI, Nazli ASGARI

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 365-381 doi: 10.1007/s11783-013-0520-5

摘要： In this work, xylene removal from waste gas streams was investigated via catalytic oxidation over Pd/carbon-zeolite and Pd/carbon-CeO nanocatalysts. Activated carbon was obtained from pine cone chemically activated using ZnCl and modified by H PO . Natural zeolite of clinoptilolite was modified by acid treatment with HCl, while nano-ceria was synthesized via redox method. Mixed supports of carbon-zeolite and carbon-ceria were prepared and palladium was dispersed over them via impregnation method. The prepared samples were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Brunauer-Emmett-Teller surface area (BET), Fourier transform infrared spectroscopy (FTIR) and thermogravimetric (TG) techniques. Characterization of nanocatalysts revealed a good morphology with an average particle size in a nano range, and confirmed the formation of nano-ceria with an average crystallite size below 60 nm. BET analysis indicated a considerable surface area for catalysts (~1000 m ·g ). FTIR patterns demonstrated that the surface groups of synthesized catalysts are in good agreement with the patterns of materials applied in catalyst synthesis. The performance of catalysts was assessed in a low-pressure catalytic oxidation pilot in the temperature range of 100°C–250°C. According to the reaction data, the synthesized catalysts have been shown to be so advantageous in the removal of volatile organic compounds (VOCs), representing high catalytic performance of 98% for the abatement of xylene at 250°C. Furthermore, a reaction network is proposed for catalytic oxidation of xylene over nanocatalysts.

关键词： Pd/carbon-CeO2     Pd/carbon-zeolite     pine cone     ZnCl2     catalytic oxidation     xylene    

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Nitrogen-doped carbon black supported Pd nanoparticles as an effective catalyst for formic acid electro-oxidation

Na SUN, Minglei WANG, Jinfa CHANG, Junjie GE, Wei XING, Guangjie SHAO

《能源前沿（英文）》 2017年 第11卷 第3期   页码 310-317 doi: 10.1007/s11708-017-0491-5

摘要： Pd nanoparticles supported on nitrogen doped carbon black (Vulcan XC-72R) with two different levels of doping were prepared by the microwave-assisted ethylene glycol reduction process and used as catalyst for the formic acid electro-oxidation (FAEO). The results indicate that the different nitrogen doping contents in Pd/N-C catalysts have a significant effect on the performance of FAEO. A higher N content facilitates the uniform dispersion of Pd nanoparticles on carbon black with narrow particle size distribution. Furthermore, the electrochemical results show that the catalyst with a higher N-doping content possesses a higher catalytic activity and a long-term stability for FAEO. The peak current density of the Pd/N-C (high) catalyst is 1.27 and 2.31 times that of the Pd/N-C (low) and homemade Pd/C-H catalyst. The present paper may provide a simple method for preparation of high-performance anode catalyst for direct formic acid fuel cells (DFAFCs).

关键词： formic acid electro-oxidation     nitrogen doped     oxidized carbon     nitrogen content    

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Pd/Fe3O4 supported on bio-waste derived cellulosic-carbon as a nanocatalyst for C–C coupling and electrocatalytic

《化学科学与工程前沿（英文）》 2022年 第16卷 第10期   页码 1514-1525 doi: 10.1007/s11705-022-2158-y

摘要： The current work describes the synthesis of a new bio-waste derived cellulosic-carbon supported-palladium nanoparticles enriched magnetic nanocatalyst (Pd/Fe3O4@C) using a simple multi-step process under aerobic conditions. Under mild reaction conditions, the Pd/Fe3O4@C magnetic nanocatalyst demonstrated excellent catalytic activity in the Hiyama cross-coupling reaction for a variety of substrates. Also, the Pd/Fe3O4@C magnetic nanocatalyst exhibited excellent catalytic activity up to five recycles without significant catalytic activity loss in the Hiyama cross-coupling reaction. Also, we explored the use of Pd/Fe3O4@C magnetic nanocatalyst as an electrocatalyst for hydrogen evolution reaction. Interestingly, the Pd/Fe3O4@C magnetic nanocatalyst exhibited better electrochemical activity compared to bare carbon and magnetite (Fe3O4 nanoparticles) with an overpotential of 293 mV at a current density of 10 mA·cm–2.

关键词： bio-waste     cellulosic-carbon     Pd/Fe3O4     Hiyama cross-coupling     hydrogen evolution reaction     recyclability    

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Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1289-1300 doi: 10.1007/s11705-023-2299-7

摘要： Environmental pollution caused by the presence of aromatic aldehydes and dyes in wastewater is a serious global concern. An effective strategy for the removal of these pollutants is their catalytic conversion, possibly to valuable compounds. Therefore, the design of efficient, stable and long-lifetime catalysts is a worthwhile research goal. Herein, we used nanofibrous carbon microspheres (NCM) derived from the carbohydrate chitin present in seafood waste, and characterized by interconnected nanofibrous networks and N/O-containing groups, as carriers for the manufacture of a highly dispersed, efficient and stable Pd nano-catalyst (mean diameter ca. 2.52 nm). Importantly, the carbonised chitin’s graphitized structure, defect presence and large surface area could promote the transport of electrons between NCM and Pd, thereby endowing NCM supported Pd catalyst with high catalytic activity. The NCM supported Pd catalyst was employed in the degradation of some representative dyes and the chemoselective hydrogenation of aromatic aldehydes; this species exhibited excellent catalytic activity and stability, as well as applicability to a broad range of aromatic aldehydes, suggesting its potential use in green industrial catalysis.

关键词： biowaste chitin     nanofibrous     palladium     nano-catalyst     catalysis    

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Enhancing the aromatic selectivity of cyclohexane aromatization by CO2 coupling

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1801-1808 doi: 10.1007/s11705-023-2325-9

摘要： Improving the aromatic selectivity in the alkane aromatization process is of great importance for its practical utilization but challenge to make because the high H/C ratio of alkanes would lead to a serious hydrogen transfer process and a large amount of light alkanes. Herein, CO2 is introduced into the cyclohexane conversion process on the HZSM-5 zeolite, which can improve the aromatic selectivity. By optimizing the reaction conditions, an improved aromatic (benzene, toluene, xylene, and C9+) selectivity of 48.2% can be obtained at the conditions of 2.7 MPa (CO2), 450 °C, and 1.7 h−1, which is better than that without CO2 (aromatic selectivity = 43.2%). In situ transmission Fourier transform infrared spectroscopy spectra illustrate that many oxygenated chemical intermediates (e.g., carboxylic acid, anhydride, unsaturated aldehydes/ketones or ketene) would be formed during the cyclohexane conversion process in the presence of CO2. 13C isotope labeling experimental results demonstrate that CO2 can enter into the aromatics through the formation of oxygenated chemical intermediates and thereby improve the aromatic selectivity. This study may open a green, economic, and promising way to improve the aromatic selectivity for alkane aromatization process.

关键词： aromatics     carbon dioxide     aromatization     coupling reaction     ZSM-5 zeolite    

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Metabolic interventions combined with CTLA-4 and PD-1/PD-L1 blockade for the treatment of tumors: mechanisms

《医学前沿（英文）》   页码 805-822 doi: 10.1007/s11684-023-1025-7

摘要： Immunotherapies based on immune checkpoint blockade (ICB) have significantly improved patient outcomes and offered new approaches to cancer therapy over the past decade. To date, immune checkpoint inhibitors (ICIs) of CTLA-4 and PD-1/PD-L1 represent the main class of immunotherapy. Blockade of CTLA-4 and PD-1/PD-L1 has shown remarkable efficacy in several specific types of cancers, however, a large subset of refractory patients presents poor responsiveness to ICB therapy; and the underlying mechanism remains elusive. Recently, numerous studies have revealed that metabolic reprogramming of tumor cells restrains immune responses by remodeling the tumor microenvironment (TME) with various products of metabolism, and combination therapies involving metabolic inhibitors and ICIs provide new approaches to cancer therapy. Nevertheless, a systematic summary is lacking regarding the manner by which different targetable metabolic pathways regulate immune checkpoints to overcome ICI resistance. Here, we demonstrate the generalized mechanism of targeting cancer metabolism at three crucial immune checkpoints (CTLA-4, PD-1, and PD-L1) to influence ICB therapy and propose potential combined immunotherapeutic strategies co-targeting tumor metabolic pathways and immune checkpoints.

关键词： CTLA-4     PD-1     PD-L1     immune checkpoint blockade (ICB)     metabolic reprogramming     combined tumor therapeutic strategies    

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PD-1/PD-L1 blockade in cervical cancer: current studies and perspectives

Yumeng Wang, Guiling Li

《医学前沿（英文）》 2019年 第13卷 第4期   页码 438-450 doi: 10.1007/s11684-018-0674-4

摘要： Cervical cancer (CC) is the fourth most commonly diagnosed female malignancy and a leading cause of cancer-related mortality worldwide, especially in developing countries. Despite the use of advanced screening and preventive vaccines, more than half of all CC cases are diagnosed at advanced stages, when therapeutic options are extremely limited and side effects are severe. Given these circumstances, new and effective treatments are needed. In recent years, exciting progress has been made in immunotherapies, including the rapid development of immune checkpoint inhibitors. Checkpoint blockades targeting the PD-1/PD-L1 axis have achieved effective clinical responses with acceptable toxicity by suppressing tumor progression and improving survival in several tumor types. In this review, we summarize recent advances in our understanding of the PD-1/PD-L1 signaling pathway, including the expression patterns of PD-1/PD-L1 and potential PD-1/PD-L1-related therapeutic strategies for CC.

关键词： PD-1     PD-L1     immune checkpoint blockade antibody     immunotherapy     cervical cancer    

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Factors affecting the formation of zeolite seed layers and the effects of seed layers on the growth ofzeolite silicalite-1 membranes

ZHANG Xiongfu, WANG Jinqu, LIU Hai′ou, WANG Anjie

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 172-177 doi: 10.1007/s11705-007-0032-6

摘要： The present study investigates the formation of silicalite-1 seed layers on a porous carbon support of 0.5 μm pore size and α-A1O supports with different pore sizes (0.1 μm and 4 μm) via the slip-casting technique. The effects of support property, seed size and solvent on the formation of seed layers were investigated in detail. The growth of silicalite-1 membranes on different seeded supports by hydrothermal synthesis was also evaluated. The scanning electron microscopy (SEM) and X-ray diffraction (XRD) characterizations indicate that a continuous seed layer can be obtained on the smooth support of 0.1 μm pore size by using any seed of 100 nm, 600 nm or 2.2 μm in size, whereas, on the coarse supports with either 0.5 μm or 4 μm pore size, a continuous seed layer cannot be formed using the above seed sizes and the same seeding time. At a longer contact time, a seed layer can also be formed using 100 nm seed on the supports with larger pore size. However, the layer is not uniform and smooth. For a hydrophobic porous carbon support, seeding ethanol suspension, which has weak polarity, favors the formation of a continuous seed layer. The seed layers and membranes grown from the smaller seed are more uniform and continuous and possess smoother surfaces than those from the larger seed. The seed layer and respective grown membrane formed from nanosized seed (100 nm) are the most uniform and compact. With this method of seeded secondary synthesis of zeolite membranes, the quality of a membrane mainly depends on the quality of the seed layer.

关键词： silicalite-1     α-A1O     growth     seeding ethanol     quality    

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Promoting effect of Zr on the catalytic combustion of methane over Pd/γ-Al

Hongbo NA,Tianle ZHU,Zhiming LIU,Yifei SUN

《环境科学与工程前沿（英文）》 2014年 第8卷 第5期   页码 659-665 doi: 10.1007/s11783-013-0613-1

摘要： The effect of Zr on the catalytic performance of Pd/γ-Al O for the methane combustion was investigated. The results show that the addition of Zr can improve the activity and stability of Pd/γ-Al O catalyst, which, based on the catalyst characterization (N adsorption, XRD, CO-Chemisorption, XPS, CH -TPR and O -TPO), is ascribed to the interaction between Pd and Zr. The active phase of methane combustion over supported palladium catalyst is the Pd /Pd mixture. Zr addition inhibits Pd aggregation and enhances the redox properties of active phase Pd / Pd . H reduction could effectively reduce the oxidation degree of Pd species and regenerate the active sites (Pd / Pd ).

关键词： Pd-Zr/Al2O3     methane     catalytic combustion     catalyst regeneration    

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Dihydroartemisinin increased the abundance of by YAP1 depression that sensitizes hepatocellular carcinoma to anti-PD

《医学前沿（英文）》 2023年 第17卷 第4期   页码 729-746 doi: 10.1007/s11684-022-0978-2

摘要： The effect of anti-programmed cell death 1 (anti-PD-1) immunotherapy is limited in patients with hepatocellular carcinoma (HCC). Yes-associated protein 1 (YAP1) expression increased in liver tumor cells in early HCC, and Akkermansia muciniphila abundance decreased in the colon. The response to anti-PD-1 treatment is associated with A. muciniphila abundance in many tumors. However, the interaction between A. muciniphila abundance and YAP1 expression remains unclear in HCC. Here, anti-PD-1 treatment decreased A. muciniphila abundance in the colon, but increased YAP1 expression in the tumor cells by mice with liver tumors in situ. Mechanistically, hepatocyte-specific Yap1 knockout (Yap1LKO) maintained bile acid homeostasis in the liver, resulting in an increased abundance of A. muciniphila in the colon. Yap1 knockout enhanced anti-PD-1 efficacy. Therefore, YAP1 inhibition is a potential target for increasing A. muciniphila abundance to promote anti-PD-1 efficacy in liver tumors. Dihydroartemisinin (DHA), acting as YAP1 inhibitor, increased A. muciniphila abundance to sensitize anti-PD-1 therapy. A. muciniphila by gavage increased the number and activation of CD8+ T cells in liver tumor niches during DHA treatment or combination with anti-PD-1. Our findings suggested that the combination anti-PD-1 with DHA is an effective strategy for liver tumor treatment.

关键词： hepatocellular carcinoma     YAP1     Akkermansia muciniphila     anti-PD-1     dihydroartemisinin     bile acid    

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CuO/zeolite catalyzed oxidation of gaseous toluene under microwave heating

Longli BO, Jianbo LIAO, Yucai ZHANG, Xiaohui WANG, Quan YANG

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 395-402 doi: 10.1007/s11783-012-0417-8

摘要： The development of a combined process of catalytic oxidation and microwave heating for treatment of toluene waste gas was described in this work. Toluene, a typical toxic volatile organic compound, was oxidized through a fixed bed reaction chamber containing zeolite-supported copper oxide (CuO/zeolite) catalyst mixed with silicon carbide (SiC), an excellent microwave-absorbing material. The target compound was efficiently degraded on the surface of the catalyst at high reaction temperature achieved by microwave-heated SiC. A set of experimental parameters, such as microwave power, air flow and the loading size of CuO etc., were investigated, respectively. The study demonstrated these parameters had critical impact on toluene degradation. Under optimal condition, 92% toluene was removed by this combined process, corresponding to an 80%–90% TOC removal rate. Furthermore, the catalyst was highly stable even after eight consecutive 6-h runs. At last, a hypothetical degradation pathway of toluene was proposed based on the experimental data obtained from gas chromatography-mass spectrum and Fourier transform infrared spectroscopy analyses.

关键词： microwave     catalytic oxidation     CuO/zeolite catalyst     silicon carbide (SiC)     toluene    

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Effects of natural zeolite and sulfate ions on the mechanical properties and microstructure of plastic

《结构与土木工程前沿（英文）》 2022年 第16卷 第1期   页码 86-98 doi: 10.1007/s11709-021-0793-x

摘要： One of the strategic materials used in earth-fill embankment dams and in modifying and preventing groundwater flow is plastic concrete (PlC). PlC is comprised of aggregates, water, cement, and bentonite. Natural zeolite (NZ) is a relatively abundant mineral resource and in this research, the microstructure, unconfined strength, triaxial behavior, and permeability of PlC made with 0%, 10%, 15%, 20%, and 25% replacement of cement by NZ were studied. Specimens of PIC-NZ were subjected to confined conditions and three different confining pressures of 200, 350, and 500 kPa were used to investigate their mechanical behavior and permeability. To study the effect of sulfate ions on the properties of PlC-NZ specimens, the specimens were cured in one of two different environments: normal condition and in the presence of sulfate ions. Results showed that increasing the zeolite content decreases the unconfined strength, elastic modulus, and peak strength of PlC-NZ specimens at the early ages of curing. However, at the later ages, increasing the zeolite content increases unconfined strength as well as the peak strength and elastic modulus. Specimens cured in the presence of sulfate ions indicated lower permeability, higher unconfined strength, elastic modulus, and peak strength due to having lower porosity.

关键词： plastic concrete     sulfate resistance     natural zeolite     triaxial compression test     SEM     permeability    

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Photocatalytic degradation of omethoate using NaY zeolite-supported TiO

Dishun ZHAO, Jialei WANG, Zhigang ZHANG, Juan ZHANG

《化学科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 206-210 doi: 10.1007/s11705-009-0053-4

摘要： The degradation of omethoate was conducted using H O as oxidant, TiO supported on NaY zeolite as photocatalyst and a 300 W lamp as light source. The effect of the calcination temperature of the photocatalyst, the amount of TiO loaded on NaY zeolite, the photocatalyst amount, the pH value and the radiation time on the degradation ratio of omethoate were investigated. The results show that TiO /NaY zeolite photocatalyst prepared by sol-gel method had good photocatalysis. The photocatalytic optimum oxidation conditions of omethoate are as follows: the calcination temperature of the photocatalyst is 550°C,the amount of TiO loaded on NaY zeolite is 35.2 wt-%, the amount of photocatalyst is 5 g/L, pH=8 and the radiation time is 180 min. Under these conditions, the removal ratio of omethoate is up to 93%.

关键词： TiO2     NaY zeolite     photocatalytic degradation     omethoate    

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A study on the catalytic performance of Pd/γ-Al

Ruizhi CHU, Xianyong WEI, Zhimin ZONG, Wenjia ZHAO

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 452-456 doi: 10.1007/s11705-010-0522-9

摘要： A series of Pd/γ-Al O hybrid catalysts were prepared by impregnation and subsequent calcination under microwave irradiation. The catalysts were used for direct synthesis of dimethylether (DME) from syngas. The results show that calcination under microwave irradiation improved both the activity and selectivity of the catalysts for DME synthesis. The optimum power of the microwave was determined to be 420 W. Under such optimum conditions, CO conversion, DME selectivity and time space yield of DME were 60.1%, 67.0%, and 21.5 mmol·mL ·h , respectively. Based on various characterizations such as nitrogen physisorption, X-ray diffraction, CO-temperature-programmed desorption, and Fourier transform infrared spectral analysis, the promotional effect of the microwave irradiation on the catalytic property was mainly attributed to both the higher dispersion of Pd and the significant increase in the adsorption on the CO-bridge of Pd. Microwave irradiation with very high power led to the increase in CO-bridge adsorption and thereby decreased the catalytic activity, whereas the coverage by metallic Pd of the active sites on acidic γ-Al O significantly occurred under microwave irradiation with very low power, resulting in a decrease in the selectivity to DME.

关键词： Pd/γ-Al2O3     direct synthesis     dimethyl ether     calcination under microwave irradiation    

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Catalytic fast pyrolysis of Kraft lignin with HZSM-5 zeolite for producing aromatic hydrocarbons

Xiangyu LI, Lu SU, Yujue WANG, Yanqing YU, Chengwen WANG, Xiaoliang LI, Zhihua WANG

《环境科学与工程前沿（英文）》 2012年 第6卷 第3期   页码 295-303 doi: 10.1007/s11783-012-0410-2

摘要： Catalytic fast pyrolysis (CFP) of Kraft lignins with HZSM-5 zeolite for producing aromatics was investigated using analytical pyrolysis methods. Two Kraft lignins were fast pyrolyzed in the absence and presence of HZSM-5 in a Curie-point pyrolyzer. Without the catalyst, fast pyrolysis of lignin predominantly produced phenols and guaiacols that were derived from the subunits of lignin. However, the presence of HZSM-5 changed the product distribution dramatically. As the SiO /Al O ratio of HZSM-5 decreased from 200 to 25 and the catalyst-to-lignin ratio increased from 1 to 20, the lignin-derived oxygenates progressively decreased to trace and the aromatics increased substantially. The aromatic yield increased considerably as the pyrolysis temperature increased from 500°C to 650°C, but then decreased with yet further increase of pyrolysis temperature. Under optimal reaction conditions, the aromatic yields were 2.0 wt.% and 5.2 wt.% for the two lignins that had effective hydrogen indexes of 0.08 and 0.35.

关键词： lignin     catalytic fast pyrolysis     HZSM-5     zeolite     aromatic hydrocarbon    

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标题 作者 时间 类型 操作

Synthesis, physicochemical characterizations and catalytic performance of Pd/carbon-zeolite and Pd/carbon-CeO

Zeinab JAMALZADEH, Mohammad HAGHIGHI, Nazli ASGARI

期刊论文

Nitrogen-doped carbon black supported Pd nanoparticles as an effective catalyst for formic acid electro-oxidation

Na SUN, Minglei WANG, Jinfa CHANG, Junjie GE, Wei XING, Guangjie SHAO

期刊论文

Pd/Fe3O4 supported on bio-waste derived cellulosic-carbon as a nanocatalyst for C–C coupling and electrocatalytic

期刊论文

Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

期刊论文

Enhancing the aromatic selectivity of cyclohexane aromatization by CO2 coupling

期刊论文

Metabolic interventions combined with CTLA-4 and PD-1/PD-L1 blockade for the treatment of tumors: mechanisms

期刊论文

PD-1/PD-L1 blockade in cervical cancer: current studies and perspectives

Yumeng Wang, Guiling Li

期刊论文

Factors affecting the formation of zeolite seed layers and the effects of seed layers on the growth ofzeolite silicalite-1 membranes

ZHANG Xiongfu, WANG Jinqu, LIU Hai′ou, WANG Anjie

期刊论文

Promoting effect of Zr on the catalytic combustion of methane over Pd/γ-Al

Hongbo NA,Tianle ZHU,Zhiming LIU,Yifei SUN

期刊论文

Dihydroartemisinin increased the abundance of by YAP1 depression that sensitizes hepatocellular carcinoma to anti-PD

期刊论文

CuO/zeolite catalyzed oxidation of gaseous toluene under microwave heating

Longli BO, Jianbo LIAO, Yucai ZHANG, Xiaohui WANG, Quan YANG

期刊论文

Effects of natural zeolite and sulfate ions on the mechanical properties and microstructure of plastic

期刊论文

Photocatalytic degradation of omethoate using NaY zeolite-supported TiO

Dishun ZHAO, Jialei WANG, Zhigang ZHANG, Juan ZHANG

期刊论文

A study on the catalytic performance of Pd/γ-Al

Ruizhi CHU, Xianyong WEI, Zhimin ZONG, Wenjia ZHAO

期刊论文

Catalytic fast pyrolysis of Kraft lignin with HZSM-5 zeolite for producing aromatic hydrocarbons

Xiangyu LI, Lu SU, Yujue WANG, Yanqing YU, Chengwen WANG, Xiaoliang LI, Zhihua WANG

期刊论文