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Petroleum Science 2024年第1期21卷 674-682页

作者： Jing He Kun zhu Wei Jiang Dong-Ao zhu Lin-Hua zhu Hai-Yan Huang wen-shuai zhu Hua-Ming Li Institute for Energy Research Jiangsu UniversityZhenjiang212013JiangsuChina College of Chemistry and Chemical Engineering Hainan Normal UniversityKey Laboratory of Water Pollution Treatment and Resource Reuse of Hainan ProvinceHaikou571158HainanChina

Synergic catalytic effect between active sites and supports greatly determines the catalytic activity for the aerobic oxidative desulfurization of fuel oils.In this work,Ni-doped Co-based bimetallic metal-organic framework(CoNi-MOF)is fabricated to disperse N-hydroxyphthalimide(NHPI),in which the whole catalyst provides plentiful synergic catalytic effect to improve the performance of oxidative desulfurization(ODS).As a bimetallic MOF,the second metal Ni doping results in the flower-like morphology and the modification of electronic properties,which ensure the exposure of NHPI and strengthen the synergistic effect of the overall catalyst.Compared with the monometallic Co-MOF and naked NHPI,the NHPI@CoNi-MOF triggers the efficient activation of molecular oxygen and improves the ODS performance without an initiator.The sulfur removal of dibenzothiophene-based model oil reaches 96.4%over the NHPI@CoNi-MOF catalyst in 8 h of reaction.Furthermore,the catalytic product of this aerobic ODS reaction is sulfone,which is adsorbed on the catalyst surface due to the difference in polarity.This work provides new insight and strategy for the design of a strong synergic catalytic effect between NHPI and bimetallic supports toward high-activity aerobic ODS materials.

关键词： Metal-organic frameworks Doped Bimetallic N-hydroxyphthalimide Aerobic processes Oxidative desulfurization

Efficient aerobic oxidative desulfurization via three-dimensional ordered macroporous tungsten-titanium oxides

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Petroleum Science 2022年第1期19卷 345-353页

作者： Ming Zhang Yu-Jie Fu Chao Wang Yan-Chen Wei Yong-Kang Gao wen-Shu Yang Lei Fan wen-shuai zhu Hua-Ming Li Institute for Energy Research School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang212013PR China Institute of Environmental Health and Ecological Security School of the Environment and Safety EngineeringJiangsu UniversityZhenjiang212013PR China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou225002PR China

A series of three-dimensional ordered macroporous(3 DOM)W-TiO_(2)catalysts have been prepared through a facile colloidal crystal template method.The prepared materials characterized in detail exhibited enhanced catalytic activity in aerobic oxidative desulfurization process.The experimental results indicated that the as-prepared materials possessed excellent 3 DOM structure,which is beneficial for the catalytic activity.The sample 3 DOM W-TiO_(2)-20 exhibited the highest activity in ODS process,and the sulfur removal can reach 98%in 6 h.Furthermore,the oxidative product was also analyzed in the reaction process.

关键词： Tungsten doped Three-dimensional ordered microporous material Titanium oxide Aerobic oxidative desulfurization Sulfur compounds

Enhanced adsorption performance for antibiotics by alcohol-solvent mediated boron nitride nanosheets

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Rare Metals 2022年第1期41卷 342-352页

作者： Hao-Feng Wu Yan-Hong Chao Guo-Hua Xia Jing Luo Duan-Jian Tao Lin-Hua zhu Gui-Ling Luo Yan Huang Ming-Qing Hua wen-shuai zhu School of Pharmacy Jiangsu UniversityZhenjiang 212013China School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China College of Chemistry and Chemical Engineering Jiangxi Normal UniversityNanchang 330022China Key Laboratory of Water Pollution Treatment and Resource Reuse of Hainan Province College of Chemistry and Chemical EngineeringHainan Normal UniversityHaikou 571158China School of Environment and Safety Engineering Jiangsu UniversityZhenjiang 212013China

The development of high-efficient adsorbents for the treatment of antibiotics from contaminated water has been of great concern.This work introduced an alcohol-solvent mediated strategy to increase the specific surface area(SSA)and porosity of hexagonal boron nitride nanosheets(BNNSs)for improving tetracycline(TC)removal efficiency.The BNNSs synthesized with the mediation of n-propanol solvent(BN-P)exhibited the largest pore volume and relatively high SSA(increased by 34%and 64%,respectively,compared with that synthesized under the mediation of water)in its structure,which in turn facilitated the mass transfer of TC molecules onto BN-P framework.The remarkable adsorption performance of BN-P,with 20%increase in equilibrium adsorption capacity and Langmuir maximum adsorption capacity of 556 mg·g^(-1),was achieved for capturing TC within just 3 h,which is mainly through p-p interaction and electrostatic force.Pseudo-second kinetics equation can well illustrate the adsorption process,while Freundlich and Langmuir isotherm models fitted the equilibrium data well.Thermodynamics study demonstrated a spontaneous exothermal adsorption process.Furthermore,the strong environmental suitability and notable recycling performance of BN-P revealed its good application prospect in removing antibiotic TC from wastewater.

关键词： Water treatment Boron nitride nanosheets Adsorption Antibiotics Solvent mediation

N-hydroxyphthalimide anchored on hexagonal boron nitride as a metal-free heterogeneous catalyst for deep oxidative desulfurization

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Petroleum Science 2022年第3期19卷 1382-1389页

作者： Lin-Jie Lu Pei-wen Wu Jing He Ming-Qing Hua Yan-Hong Chao Ning Yang Lin-Lin Chen Wei Jiang Lei Fan Hong-Bing Ji wen-shuai zhu School of Chemistry and Chemical Engineering Institute for Energy ResearchJiangsu UniversityZhenjiangJiangsu212013PR China School of Pharmacy Jiangsu UniversityZhenjiangJiangsu212013PR China Yangzhou University YangzhouJiangsu225002PR China Fine Chemical Industry Research Institute School of ChemistrySun Yat-sen UniversityGuangzhouGuangdong510275PR China

A metal-free N-hydroxyphthalimide/hexagonal boron nitride(NHPI/h-BN)catalytic system was developed for deep oxidative desulfurization(ODS)of fuel oils.Detailed experiments find that the heterogenization process of loading NHPI on h-BN not only benefits to the dispersion and utilization of NHPI,but also can significantly promote the catalytic performance.By employing NHPI/h-BN as the catalyst,azodiisobutyronitrile(AIBN)as the metal-free initiator,a 95%conversion of dibenzothiophene(DBT)can be acquired under the reaction conditions of 120°C and atmospheric pressure with molecular oxygen(O_(2))as oxidant.Moreover,the heterogenization is convenient for the regeneration of the catalyst with>94%DBT conversion after being recycled seven times.Characterizations illustrate that the promoted catalytic activity along with the regenerability originate from the interactions between NHPI and h-BN.The catalytic mechanism study shows that molecular oxygen is readily activated by the NHPI/h-BN to form a superoxide radical(O_(2)^(·-)),which oxidize DBT to DBTO2 for desulfurization.

关键词： N-hydroxyphthalimide Hexagonal boron nitride Oxidative desulfurization Heterogeneous catalysis

Catalytic oxidation of pentanethiol on basic nitrogen doped carbon hollow spheres derived from waste tires

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Petroleum Science 2022年第4期19卷 1888-1896页

作者： Jing Luo wen-Feng Zhang Yan-Chen Wei Ji-Xing Liu Chao Wang Yi-Ru Zou Hai-Tao Ju Li-Ping Mu Yan-Hong Chao Hong-Bing Ji wen-shuai zhu School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang212013JiangsuChina School of Materials Science and Engineering Jiangsu UniversityZhenjiang212013JiangsuChina School of the Environment and Safety Engineering Jiangsu UniversityZhenjiang212013JiangsuChina College of Chemical Engineering and Environment State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingChangping102249BeijingChina School of Chemistry Sun Yat-Sen UniversityGuangzhou510275GuangdongChina

A series of basic nitrogen doped carbon hollow spheres(p-N-C) catalysts derived from waste tires were prepared by a green, facile and environmental “leavening” strategy for the catalytic oxidation of pentanethiol. Compared to pristine carbon, the p-N-C has a higher surface curvature conducive to the enrichment of substrates, leading to an excellent catalytic performance. This increased surface curvature of p-N-C was fabricated on the synergistic effect of two foaming agents((NH4)2 C2 O4 and NaHCO3), and the released gas also endows the spherical shell of p-N-C with a hierarchical porous structure, promoting the accessibility of active sites with pentanethiol. Pyridine-like and pyrrolic-like nitrogen atoms were investigated as reactive sites on the p-N-C to accelerate the electron transfer from sulfur to active surface oxygen and enhance the adsorption/oxidation process. As a result, the optimal p-N-C catalyst exhibits superior adsorption and oxidation performance(99.9%) of pentanethiol, outperforming the “unleavened”catalyst(20.8%). This work offers a new avenue for the fabrication of highly efficient materials for the desulfurization of fuel.

关键词： Carbon hollow spheres Nitrogen-doping Waste tires Leavening strategy Pentanethiol

Active phase morphology engineering of NiMo/Al2O3 through La introduction for boosting hydrodesulfurization of 4,6-DMDBT

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Petroleum Science 2023年第2期20卷 1231-1237页

作者： Ji-Xing Liu Xiang-Qi Liu Ri-Xin Yan Ling-Feng Ji Hui-Fang Cheng Hui Liu Yan Huang Ming-Qing Hua Hua-Ming Li wen-shuai zhu School of Chemistry and Chemical Engineering and Institute for Energy Research Jiangsu UniversityZhenjiangJiangsu 212013China State Key Laboratory of Heavy Oil Processing and Beijing Key Lab of Oil&Gas Pollution Control China University of PetroleumBeijing 102249China State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalianLiaoning 116024China

Herein,we designed and constructed a mesoporous LaAlOx via a solvent evaporation induced self-assembly protocol.The structure and physicochemical property of the corresponding NiMo supported catalyst was analyzed by a set of characterizations,and its catalytic activity was investigated for hydrodesulfurization(HDS)of 4,6-dimethyldibenzothiophene.It has confirmed that the incorporation of La profoundly facilitate the generation of“Type II”NiMoS phase by weakening the interaction of Mo–O–Al leakage and promoting the sulfidation of both Ni and Mo oxides as well as changing the morphology of Ni promoted MoS2 slabs,thereafter boosting the HDS performance substantially.The finding here may contribute to the fundamental understanding of structure-activity in ultra-deep desulfurization and inspire the advancement of highly-efficient HDS catalyst in future.

关键词： NiMo supported Catalyst LaAlOx composites Hydrodesulfurization Morphology Reaction kinetics

Aerobic oxidative desulfurization via magnetic mesoporous silica-supported tungsten oxide catalysts

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Petroleum Science 2020年第5期17卷 1422-1431页

作者： Wei Jiang Xiang Gao Lei Dong Jin Xiao Lin-Hua zhu Guang-Ying Chen Su-Hang Xun Chong Peng wen-shuai zhu Hua-Ming Li Institute for Energy Research School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang 212013People’s Republic of China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013People’s Republic of China School of Chemistry and Chemical Engineering Hainan Normal UniversityHaikou 571158HainanPeople’s Republic of China Dalian Research Institute of Petroleum and Petrochemicals SINOPECNankai Road 96 of Lushunkou CityDalian 116045People’s Republic of China

It is usually difficult to remove dibenzothiophenes from diesel fuels by oxidation with molecular oxygen as an oxidant.In the study,tungsten oxide was supported on magnetic mesoporous silica by calcination to form a magnetically separable catalyst for oxidative desulfurization of diesel fuel.By tuning different calcining temperatures,the catalyst calcined at 500℃showed a high catalytic activity with molecular oxygen as the oxidant.Under optimal reaction conditions,the sulfur removal of DBT reached 99.9%at 120℃after 8 h.Furthermore,the removals of 4-methyldibenzothiophene and 4,6-dimethyldibenzothiophene could also get up to 98.2%and 92.3%under the same conditions.The reaction mechanism was explored by selective quenching experiments and FT-IR spectra.

关键词： Oxidative desulfurization Molecular oxygen Magnetic separation Mesoporous structure Tungsten oxide

Insight into the oxidative desulfurization of high-sulfur petroleum coke under mild conditions:a journey of vanadium-substituted Dawson-type phosphotungstic acid

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Petroleum Science 2021年第3期18卷 983-993页

作者： Fu-Min Li Ming-Qing Hua Yan-Chen Wei Ji-Xing Liu Jia-Hong Gong Chao Wang Pei-wen Wu Yan Huang Hua-Ming Li wen-shuai zhu School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China School of the Environment and Safety Engineering Jiangsu UniversityZhenjiang 212013China

High-sulfur petroleum coke(HSPC),that is a by-product from slag oil in the coking process of refning,shows versatility values in practical applications and,however,concentrates the majority of organic sulfur.Herein,we design and construct a highly efective CTAB@HPA composites to be explored for the catalytic oxidative desulfurization of HSPC under mild conditions using hydrogen peroxide as the oxidant and 1-butyl-3-methylimidazole tetrafuoroborate ionic liquid as the extractant.The results demonstrate that the sulfur content of HSPC could be strikingly reduced from 4.46 wt%to 2.48 wt%under 60℃ and atmospheric pressure,and that the organic sulfur in HSPC is mainly oxidized to sulfoxide,sulfone and sulfate,which latter can be directly separated from petroleum coke.Moreover,the efect of reaction conditions on the desulfurization performance of HSPC as well as the catalytic oxidation reaction kinetic of HSPC desulfurization was systematically investigated.Furthermore,a mechanism for the oxidative desulfurization of HSPC over CTAB@HPA catalysts was proposed.Therefore,this work provides new insight into how to construct active catalysts for the desulfurization of HSPC under mild conditions.

关键词： High-sulfur petroleum coke Dawson-type phosphotungstic acid Oxidative desulfurization Mild conditions Sulfate

ALKBH5 suppresses autophagic flux via N6-methyladenosine demethylation of ZKSCAN3 mRNA in acute pancreatitis

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World Journal of Gastroenterology 2024年第12期30卷 1764-1776页

作者： Tao Zhang shuai zhu Geng-wen Huang Department of General Surgery Xiangya HospitalCentral South UniversityChangsha 410005HunanChina. National Clinical Research Center for Geriatric Disorders Xiangya HospitalCentral South UniversityChangsha 410005HunanChina.

BACKGROUND Increasing evidence has demonstrated that N6-methyladenosine(m6A)RNA modification plays an essential role in a wide range of pathological conditions.Impaired autophagy is a critical hallmark of acute pancreatitis(AP).AIM To explore the role of the m6A modification of ZKSCAN3 in the regulation of autophagy in AP.METHODS The AP mouse cell model was established by cerulein-treated mouse pancreatic acinar cells(MPC-83),and the results were confirmed by the levels of amylase and inflammatory factors.Autophagy activity was evaluated by specific identification of the autophagy-related microstructure and the expression of autophagy-related genes.ZKSCAN3 and ALKBH5 were knocked down to study the function in AP.A m6A RNA binding protein immunoprecipitation assay was used to study how the m6A modification of ZKSCAN3 mRNA is regulated by ALKBH.RESULTS The increased expression of amylase and inflammatory factors in the supernatant and the accumulation of autophagic vacuoles verified that the AP mouse cell model was established.The downregulation of LAMP2 and upregulation of LC3-II/I and SQSTM1 demonstrated that autophagy was impaired in AP.The expression of ZKSCAN3 was upregulated in AP.Inhibition of ZKSCAN3 increased the expression of LAMP2 and decreased the expression of the inflammatory factors,LC3-II/I and SQSTM1.Furthermore,ALKBH5 was upregulated in AP.Knockdown of ALKBH5 downregulated ZKSCAN3 expression and restored decreased autophagic flux in AP.Notably,the bioinformatic analysis revealed 23 potential m6A modification sites on ZKSCAN3 mRNA.The m6A modification of ZKSCAN3 mRNA was significantly decreased in AP.Knockdown of ALKBH5 increased the modification of ZKSCAN3 mRNA,which confirmed that ALKBH5 upregulated ZKSCAN3 expression in a m6A-dependent manner.CONCLUSION ALKBH5 inhibits autophagic flux through m6A demethylation of ZKSCAN3 mRNA in AP,thereby aggravating the severity of the disease.

关键词： Acute pancreatitis Autophagy ZKSCAN3 N6-methyladenosine ALKBH5

Histological Features of Uterine Myometrial Dysfunction:Possible Involvement of Localized Inflammation

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Current Medical Science 2024年第3期44卷 633-641页

作者： Sheng-lan zhu Hui-ting ZHANG Yuan-yuan DU Yi JIANG Shao-shuai WANG wen-cheng DING Ling FENG National Clinical Research Center for Obstetrics and Gynecology Tongji HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430030China Department of Obstetrics and Gynecology Tongji HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430030China

Objective The latest perspective suggests that elevated levels of inflammation and cytokines are implicated in atonic postpartum hemorrhage.Lipopolysaccharide(LPS)has been widely used to induce inflammation in animal models.Therefore,this study aimed to induce uterine inflammation using LPS to investigate whether local inflammation triggers dysfunction and atrophy in the myometrium,as well as the potential underlying molecular mechanisms involved.Methods In vivo,an animal model was established by intraperitoneal injection of 300μg/kg LPS in rats on gestational day 21.Hematoxylin-eosin(H&E)staining and Masson staining were employed to determine morphological changes in the rat uterine smooth muscle.Enzyme-linked immunosorbent assay(ELISA)was used to detect inflammatory cytokines.Immunohistochemistry,tissue fluorescence,and Western blotting were conducted to assess the expression levels of the uterine contraction-related proteins Toll-like receptor 4(TLR4)and the nuclear factor kappa-B(NF-κB)signaling pathway.In vitro,human uterine smooth muscle cells(HUtSMCs)were exposed to 2μg/mL LPS to further elucidate the involvement of the TLR4/NF-κB signaling pathway in LPS-mediated inflammation.Results In this study,LPS induced uterine myometrial dysfunction in rats,leading to a disorganized arrangement,a significant increase in collagen fiber deposition,and widespread infiltration of inflammatory cells.In both in vivo animal models and in vitro HUtSMCs,LPS elevated IL-6,IL-1β,and TNF-αlevels while concurrently suppressing the expression of connexin 43(Cx43)and oxytocin receptor(OXTR).Mechanistically,the LPS-treated group exhibited TLR4 activation,and the phosphorylation levels of p65 and IκBαwere notably increased.Conclusion LPS triggered the TLR4/NF-κB signaling pathway,inducing an inflammatory response in the myometrium and leading to uterine myometrial dysfunction and uterine atony.

关键词： lipopolysaccharide inflammatory response TLR4 NF-κB myometrium