The MoS_(2)-based materials are a vital class of heterogeneous catalysts for the hydrodeoxygenation of lignin and its model compounds to produce value-added chemicals especially because of their unique selectivity to ...The MoS_(2)-based materials are a vital class of heterogeneous catalysts for the hydrodeoxygenation of lignin and its model compounds to produce value-added chemicals especially because of their unique selectivity to aromatics.The rational design of MoS_(2)-based catalyst greatly depends on the comprehensive understanding of its structure-activity relationship.However,an intensive summary and critical analysis are still scarce to date.In this review,we attempt to provide an in-depth understanding of the interplay of structure,catalysis,and stability of MoS_(2)-based catalysts for lignin hydrodeoxygenation.The recognition of intrinsic active sites on MoS_(2) structure was firstly discussed,followed by the illustration of MoS_(2)-catalyzed hydrodeoxygenation structural models.Afterward,based on the studies on the MoS_(2)-catalyzed lignin model compounds hydrodeoxygenation,the current active site modification strategies including structural modification of monometallic MoS_(2) catalysts and collaborative modification were summarized and emphatically discussed,which aims to elucidate the structure-activity relationship at the atomic-level.The deactivation mechanism and stabilization strategies were also illustrated to provide instructive suggestion for the rational design of efficient and stable MoS_(2)-based catalysts.Finally,the real lignin depolymerization over MoS_(2)-based catalysts was summarized to point out the advantages and difficulties.This review attempts to highlight the remaining challenges and provide some perspectives for the future development of MoS_(2)-based catalysts for lignin hydrodeoxygenation.展开更多
Hydrodeoxygenation(HDO) is an effective alternative to produce value-added chemicals and liquid fuels by removing oxygen from lignin-derived compounds. Sulfide catalysts have been proved to have good activity for th...Hydrodeoxygenation(HDO) is an effective alternative to produce value-added chemicals and liquid fuels by removing oxygen from lignin-derived compounds. Sulfide catalysts have been proved to have good activity for the HDO and particularly high selectivity to phenolic products. Herein, we presented a novel way to prepare the layered structure sulfide catalysts(MgFeMo-S) derived from MgFe hydrotalcites via the intercalation of Mo in consideration of the memory effect of the calcined hydrotalcite. By varying the Mg/Fe mole ratio, a series of MgFeMo-S catalysts were successfully prepared and characterized by nitrogen adsorption/desorption isotherms, X-ray diffraction(XRD), transmission electron microscopy(TEM),and inductively coupled plasma optical emission spectrometer(ICP-OES). The characterization results indicated that the MgFeMo-S catalyst has retained the unique layered structure, which can facilitate uniform dispersion of the MoS2 species on both the surface and interlayer of the catalysts. For the HDO of eugenol, the Mg1Fe2Mo-S catalysts exhibited the best HDO activity among all the catalysts due to its higher active metal contents and larger pore size. The HDO conversion was 99.6% and the yield of phenolics was 63.7%, under 5 MPa initial H2 pressure(measured at RT) at 300 ℃ for 3 h. More importantly,MoS2 species deposited on the interlayer galleries in the MgFeMo-S catalysts resulted in dramatically superior HDO activity to MoS2/Mg1Fe2-S catalyst. Based on the mechanism investigation for eugenol, the HDO reaction route of eugenol under sulfide catalytic system has been proposed for the first time. Further applicability of the catalyst on HDO of more lignin-derived compounds was operated, which showed good HDO activity and selectivity to produce aromatic products.展开更多
研究旨在建立一种猪伪狂犬病病毒(PRV)的探针法荧光定量检测方法。选用PRV gE基因为靶基因,比对不同野毒在该基因的保守区域设计特异性引物和探针,构建PRV gE基因片段的重组质粒作为标准品,对该方法的反应体系和条件进行优化,并进一步...研究旨在建立一种猪伪狂犬病病毒(PRV)的探针法荧光定量检测方法。选用PRV gE基因为靶基因,比对不同野毒在该基因的保守区域设计特异性引物和探针,构建PRV gE基因片段的重组质粒作为标准品,对该方法的反应体系和条件进行优化,并进一步评估该方法的敏感性、特异性和稳定性,最后与商品化试剂盒同时检测临床样本,比较符合率。结果表明,该研究建立的T a q M a n荧光定量P C R检测方法的最佳反应条件为上下游引物和探针量分别为0.2μm o l/L和0.05μm o l/L,最佳退火温度为58℃。该方法具有良好的特异性,对PRV Bartha-k61疫苗株、猪流行性腹泻病毒(PEDV)、猪细小病毒(PPV)、猪A群轮状病毒(PoRV)、猪德尔塔冠状病毒(PDCoV)、猪传染性胃肠炎病毒(TGEV)、猪链球菌(S.suis)、猪源大肠杆菌(E.coli)、猪源巴氏杆菌(P.multocida)、猪霍乱沙门氏菌(S.choleraesuis)和葡萄球菌(S.aureus)等11个菌毒种均无非特异性扩增。该方法的最低检测限为3.92 copies/μL。重复性试验结果显示,组内和组间变异系数均≤2%。与商品化的荧光定量PCR检测试剂盒比较,符合率均为100%(n=50)。综上所述,该研究建立了一种灵敏高效的检测PRV野毒株的TaqMan荧光定量PCR方法,该方法可以成为猪伪狂犬病早期快速诊断和流行病学调查的一种可靠的技术手段。展开更多
As one of the main oxygen-containing organic products generated from the hydrothermal conversion of biomass,levulinic acid(LA)has the potential to be further upgraded.This work investigated the steam reforming(SR)proc...As one of the main oxygen-containing organic products generated from the hydrothermal conversion of biomass,levulinic acid(LA)has the potential to be further upgraded.This work investigated the steam reforming(SR)process of biomass-derived LA to produce H_(2).A series of Ni catalysts supported by various spinels were synthesized via co-precipitation and impregnation.The Ni active metal dispersed well on the NiAl_(2)O_(4)catalyst with high specific surface area,thereby exhibiting high catalytic activity.Among all the catalysts tested,15Ni/NiAl_(2)O_(4)showed the best performance for SR of LA,resulting in high carbon conversion of 96.3%,H_(2)yield of 92.8%,and H_(2)concentration of 67.9%at a reaction temperature of 800℃.Additionally,the influences of reaction temperature,steam-to-carbon ratio(S/C),and liquid hourly space velocity(LHSV)were also examined.Moreover,during the 40-h continuous SR process of LA,the 15Ni/NiAl_(2)O_(4)catalyst maintained its outstanding catalytic activity.This study provides an encouraging route for upgrading biomass-derived LA into eco-friendly and high-value fuels,thereby advancing the sustainability of the biomass refining process.展开更多
Volatile organic compounds(VOCs)with high toxicity and carcinogenicity are emitted from kinds of industries,which endanger human health and the environment.Adsorption is a promising method for the treatment of VOCs du...Volatile organic compounds(VOCs)with high toxicity and carcinogenicity are emitted from kinds of industries,which endanger human health and the environment.Adsorption is a promising method for the treatment of VOCs due to its low cost and high efficiency.In recent years,activated carbons,zeolites,and mesoporous materials are widely used to remove VOCs because of their high specific surface area and abundant porosity.However,the hydrophilic nature and low desorption rate of those materials limit their commercial application.Furthermore,the adsorption capacities of VOCs still need to be improved.Porous organic polymers(POPs)with extremely high porosity,structural diversity,and hydrophobic have been considered as one of the most promising candidates for VOCs adsorption.This review generalized the superiority of POPs for VOCs adsorption compared to other porous materials and summarized the studies of VOCs adsorption on different types of POPs.Moreover,the mechanism of competitive adsorption between water and VOCs on the POPs was discussed.Finally,a concise outlook for utilizing POPs for VOCs adsorption was discussed,noting areas in which further work is needed to develop the next-generation POPs for practical applications.展开更多
基金supported by the National Natural Science Foundation of China(22178258,21975181)。
文摘The MoS_(2)-based materials are a vital class of heterogeneous catalysts for the hydrodeoxygenation of lignin and its model compounds to produce value-added chemicals especially because of their unique selectivity to aromatics.The rational design of MoS_(2)-based catalyst greatly depends on the comprehensive understanding of its structure-activity relationship.However,an intensive summary and critical analysis are still scarce to date.In this review,we attempt to provide an in-depth understanding of the interplay of structure,catalysis,and stability of MoS_(2)-based catalysts for lignin hydrodeoxygenation.The recognition of intrinsic active sites on MoS_(2) structure was firstly discussed,followed by the illustration of MoS_(2)-catalyzed hydrodeoxygenation structural models.Afterward,based on the studies on the MoS_(2)-catalyzed lignin model compounds hydrodeoxygenation,the current active site modification strategies including structural modification of monometallic MoS_(2) catalysts and collaborative modification were summarized and emphatically discussed,which aims to elucidate the structure-activity relationship at the atomic-level.The deactivation mechanism and stabilization strategies were also illustrated to provide instructive suggestion for the rational design of efficient and stable MoS_(2)-based catalysts.Finally,the real lignin depolymerization over MoS_(2)-based catalysts was summarized to point out the advantages and difficulties.This review attempts to highlight the remaining challenges and provide some perspectives for the future development of MoS_(2)-based catalysts for lignin hydrodeoxygenation.
基金supported by the National Natural Science Foundation of China (Grant nos. 21503144, 21406165, 51506147, 21376239)Major Projects of the National Natural Science Foundation of China (21690083)Tianjin Research Program of Application Foundation and Advanced Technique (Nos.16JCQNJC05400, 15JCQNJC08500)
文摘Hydrodeoxygenation(HDO) is an effective alternative to produce value-added chemicals and liquid fuels by removing oxygen from lignin-derived compounds. Sulfide catalysts have been proved to have good activity for the HDO and particularly high selectivity to phenolic products. Herein, we presented a novel way to prepare the layered structure sulfide catalysts(MgFeMo-S) derived from MgFe hydrotalcites via the intercalation of Mo in consideration of the memory effect of the calcined hydrotalcite. By varying the Mg/Fe mole ratio, a series of MgFeMo-S catalysts were successfully prepared and characterized by nitrogen adsorption/desorption isotherms, X-ray diffraction(XRD), transmission electron microscopy(TEM),and inductively coupled plasma optical emission spectrometer(ICP-OES). The characterization results indicated that the MgFeMo-S catalyst has retained the unique layered structure, which can facilitate uniform dispersion of the MoS2 species on both the surface and interlayer of the catalysts. For the HDO of eugenol, the Mg1Fe2Mo-S catalysts exhibited the best HDO activity among all the catalysts due to its higher active metal contents and larger pore size. The HDO conversion was 99.6% and the yield of phenolics was 63.7%, under 5 MPa initial H2 pressure(measured at RT) at 300 ℃ for 3 h. More importantly,MoS2 species deposited on the interlayer galleries in the MgFeMo-S catalysts resulted in dramatically superior HDO activity to MoS2/Mg1Fe2-S catalyst. Based on the mechanism investigation for eugenol, the HDO reaction route of eugenol under sulfide catalytic system has been proposed for the first time. Further applicability of the catalyst on HDO of more lignin-derived compounds was operated, which showed good HDO activity and selectivity to produce aromatic products.
文摘研究旨在建立一种猪伪狂犬病病毒(PRV)的探针法荧光定量检测方法。选用PRV gE基因为靶基因,比对不同野毒在该基因的保守区域设计特异性引物和探针,构建PRV gE基因片段的重组质粒作为标准品,对该方法的反应体系和条件进行优化,并进一步评估该方法的敏感性、特异性和稳定性,最后与商品化试剂盒同时检测临床样本,比较符合率。结果表明,该研究建立的T a q M a n荧光定量P C R检测方法的最佳反应条件为上下游引物和探针量分别为0.2μm o l/L和0.05μm o l/L,最佳退火温度为58℃。该方法具有良好的特异性,对PRV Bartha-k61疫苗株、猪流行性腹泻病毒(PEDV)、猪细小病毒(PPV)、猪A群轮状病毒(PoRV)、猪德尔塔冠状病毒(PDCoV)、猪传染性胃肠炎病毒(TGEV)、猪链球菌(S.suis)、猪源大肠杆菌(E.coli)、猪源巴氏杆菌(P.multocida)、猪霍乱沙门氏菌(S.choleraesuis)和葡萄球菌(S.aureus)等11个菌毒种均无非特异性扩增。该方法的最低检测限为3.92 copies/μL。重复性试验结果显示,组内和组间变异系数均≤2%。与商品化的荧光定量PCR检测试剂盒比较,符合率均为100%(n=50)。综上所述,该研究建立了一种灵敏高效的检测PRV野毒株的TaqMan荧光定量PCR方法,该方法可以成为猪伪狂犬病早期快速诊断和流行病学调查的一种可靠的技术手段。
基金State Key Laboratory of Clean Energy Utilization(Open Fund Project No.ZJUCEU2021004).
文摘As one of the main oxygen-containing organic products generated from the hydrothermal conversion of biomass,levulinic acid(LA)has the potential to be further upgraded.This work investigated the steam reforming(SR)process of biomass-derived LA to produce H_(2).A series of Ni catalysts supported by various spinels were synthesized via co-precipitation and impregnation.The Ni active metal dispersed well on the NiAl_(2)O_(4)catalyst with high specific surface area,thereby exhibiting high catalytic activity.Among all the catalysts tested,15Ni/NiAl_(2)O_(4)showed the best performance for SR of LA,resulting in high carbon conversion of 96.3%,H_(2)yield of 92.8%,and H_(2)concentration of 67.9%at a reaction temperature of 800℃.Additionally,the influences of reaction temperature,steam-to-carbon ratio(S/C),and liquid hourly space velocity(LHSV)were also examined.Moreover,during the 40-h continuous SR process of LA,the 15Ni/NiAl_(2)O_(4)catalyst maintained its outstanding catalytic activity.This study provides an encouraging route for upgrading biomass-derived LA into eco-friendly and high-value fuels,thereby advancing the sustainability of the biomass refining process.
基金supported by the National Key R&D Pro-gram of China(Nos.2019YFC1904100,2019YFC1904102,2019YFC1903902,and 2016YFC0205300)the National En-gineering Laboratory for Mobile Source Emission Control Technology of China(No.NELMS2017A03)+3 种基金the Natural Na-tional Science Foundation of China(Nos.21503144,21690083)Tianjin Research Program of Ecological Environmental Treat-ment(Nos.18ZXSZSF00210,18ZXSZSF00060)the Tianjin Research Program of Application Foundation and Advanced Technique(No.16JCQNJC05400)Major Science and Tech-nology Project for Ecological Environment Management in Tianjin(No.18ZXSZSF00210)。
文摘Volatile organic compounds(VOCs)with high toxicity and carcinogenicity are emitted from kinds of industries,which endanger human health and the environment.Adsorption is a promising method for the treatment of VOCs due to its low cost and high efficiency.In recent years,activated carbons,zeolites,and mesoporous materials are widely used to remove VOCs because of their high specific surface area and abundant porosity.However,the hydrophilic nature and low desorption rate of those materials limit their commercial application.Furthermore,the adsorption capacities of VOCs still need to be improved.Porous organic polymers(POPs)with extremely high porosity,structural diversity,and hydrophobic have been considered as one of the most promising candidates for VOCs adsorption.This review generalized the superiority of POPs for VOCs adsorption compared to other porous materials and summarized the studies of VOCs adsorption on different types of POPs.Moreover,the mechanism of competitive adsorption between water and VOCs on the POPs was discussed.Finally,a concise outlook for utilizing POPs for VOCs adsorption was discussed,noting areas in which further work is needed to develop the next-generation POPs for practical applications.