SAPO-5 zeolite supported RuMn was a highly efficient catalyst for the aqueous-phase selective hydrodeoxygenation of guaiacol to cyclohexanol.The optimal catalyst achieved a high cyclohexanol yield of 93.7%at full guai...SAPO-5 zeolite supported RuMn was a highly efficient catalyst for the aqueous-phase selective hydrodeoxygenation of guaiacol to cyclohexanol.The optimal catalyst achieved a high cyclohexanol yield of 93.7%at full guaiacol conversion under mild conditions,with a high TOF of 920 h^(-1).Moreover,the catalyst displayed remarkable performance for the hydrogenation of phenol to cyclohexanol,where a 100%yield of cyclohexanol was obtained at a phenol-to-Ru molar ratio of about 17900.In particular,the catalyst exhibited excellent recyclability and could be recycled for 20 times without obvious activity loss.The as-prepared RuMn/SAPO-5 catalyst exhibited higher performance than most of the reported Rubased catalysts.展开更多
Rational design of Zn-containing HZSM-5 zeolite(Zn/HZSM-5)with high reactivity and excellent aromatization performance for olefin aromatization is crucially desired.We develop a new and uncomplicated method to synthes...Rational design of Zn-containing HZSM-5 zeolite(Zn/HZSM-5)with high reactivity and excellent aromatization performance for olefin aromatization is crucially desired.We develop a new and uncomplicated method to synthesize Zn/HZSM-5(IMX/Z5)with superior aromatization performance in the paper.Compared to incipient wetness impregnation(IMP/Z5)and mechanical mixing(MIX/Z5),the asprepared IMX/Z5 presents a higher amount of surface ZnOH^(+)species(2.87%)while keeping identical bulk zinc content.As a result,more surface ZnOH^(+)favor both the aromatization of 1-hexene and cyclohexane dehydrogenation.For the two olefin aromatization pathways(hydrogen transfer and dehydrogenation),it is the first time found both the hydrogen transfer ability and the dehydrogenation ability increase linearly with the amount of surface ZnOH^(+)species while keeping identical bulk zinc content.We believe that the linear relationships are essential to design next generation olefin aromatization catalysts.展开更多
The oxidative desulphurization(ODS)has become mainly popular by rapid catalytic oxidation of dibenzothiophene(DBT)relied on efficient heterogeneous catalyst,V-based catalytic active species were regarded as the potent...The oxidative desulphurization(ODS)has become mainly popular by rapid catalytic oxidation of dibenzothiophene(DBT)relied on efficient heterogeneous catalyst,V-based catalytic active species were regarded as the potential option in the activity-preferred ODS systems.Herein,we reported the redispersion of vanadium oxide(VO_(χ))on the mesoporous silica modified with manganese oxide(Mn_(3)O_(4)) through one progressive insertion approach of metal oxides in the silica.Impressively,mesoporeencaged vanadium-manganese oxides in the silica(VMn-MS)as the admirable output of excellent ODS catalyst was demonstrated compared to other monometal-modified counterparts and one-pot implanted one.The characterization results revealed the post-implanted VO_(χ) species not only deposited around the pre-covered Mn_(3)O_(4) on the mesoporous surface but also inserted the surface layer of Mn_(3)O_(4) inducing the amorphous evolution of aggregated Mn_(3)O_(4) and the reconstruction of final active sites.This integrated approach made the reconstructed active species afford more exposed catalytic sites and the tailored surface redox cycles owing to the electronic communication of V-Mn.The catalytic results demonstrated the excellent catalytic desulphurization efficiency(~100%)during 60 min at 80℃,which made the sulphur content reduce to 6 mg·L^(-1),remarkably superior to other comparative samples.The outstanding catalytic performance of VMn-MS catalyst can be ascribed to the synergistic effect of V-Mn dual metals rendering two different reaction pathways,which includes free-radical reaction and ring-forming reaction,where Mn site acted as active center triggering reactive free radicals which could be further optimized by surrounded V sites around Mn sites to promote the ODS process.展开更多
目的探讨经门静脉胰岛细胞移植(PIT)后,细胞间粘附分子-1(ICAM-1)的表达与移植免疫排斥反应的关系,为胰岛细胞移植术后排斥反应的临床治疗提供理论依据。方法30只Wistar糖尿病大鼠随机分为三组,A组:糖尿病模型组(n=10),不做任何处理;B组...目的探讨经门静脉胰岛细胞移植(PIT)后,细胞间粘附分子-1(ICAM-1)的表达与移植免疫排斥反应的关系,为胰岛细胞移植术后排斥反应的临床治疗提供理论依据。方法30只Wistar糖尿病大鼠随机分为三组,A组:糖尿病模型组(n=10),不做任何处理;B组:生理盐水组(n=10),采用腹腔注射生理盐水2ml/d;C组:免疫抑制剂组(n=10),采用腹腔注射CsA(3mg·kg^-1.d^-1)+MMF(20mg·kg^-1.d^-1);全部采取SD大鼠胰岛细胞→Wistar大鼠糖尿病动物模型。观察:①各组胰岛细胞移植术后第1、4、7、10、30、60天大鼠外周血血糖的变化;②流式细胞仪(Elite Coulter Company US)技术检测胰岛细胞移植术后外周血粘附分子ICAM-1的表达情况;③免疫组化方法检测各组胰岛细胞移植术后第10、60天,肝脏中ICAM-1的表达水平。结果①血糖值变化:术前各组间血糖值比较无统计学差异(P=0.669);B、C组血糖在术后第7或10天达最低水平,之后逐渐上升;任何两组间比较有统计学差异。②外周血ICAM-1的表达情况:术前各组间ICAM-1值比较无统计学差异(P=0.754);术后C组在第7或10天达最低水平,以后逐渐上升,最后接近B组水平;任何两组间比较有统计学差异。③肝脏粘附分子表达:术后10d和术后60d比较:A组(P=0.816)无统计学差异,B组(P=0.855)无统计学差异,C组(P=0.000)有统计学差异;术后10d:任何两组间均存在统计学差异(P<0.05);术后60d:B组与C组无统计学差异,A组同任何组均存在统计学差异(P<0.05)。结论PIT后粘附分子的变化与免疫排斥反应的发生有很大的相关性,进而和移植物功能有一定的相关性,且粘附分子表达水平的升高可以预示免疫排斥反应的发生。展开更多
利用ZSM-5分子筛对污水中的NH_(3)-N进行吸附脱除。通过改变吸附条件对污水中NH_(3)-N的去除效果进行探究分析。结果表明,在25℃、pH为7的溶液中,使用1 g ZSM-5分子筛吸附氨氮废水30 min时效果最佳。为探究其吸附机理,对ZSM-5分子筛进...利用ZSM-5分子筛对污水中的NH_(3)-N进行吸附脱除。通过改变吸附条件对污水中NH_(3)-N的去除效果进行探究分析。结果表明,在25℃、pH为7的溶液中,使用1 g ZSM-5分子筛吸附氨氮废水30 min时效果最佳。为探究其吸附机理,对ZSM-5分子筛进行等温吸附、吸附热力学、吸附动力学研究。结果表明,其等温吸附更符合Langmuir模型,吸附过程为吸热过程,其吸附动力学更符合Lagergren准二级模型。为提升ZSM-5分子筛的吸附效果,分别使用盐酸、氢氧化钠、氯化钠对其进行改性。结果表明,改性后的分子筛性能均有不同程度的提升,其中0.5 mol/L的氢氧化钠改性后的分子筛吸附50 mg/L的氨氮废水,处理后氨氮浓度降至3.5 mg/L。展开更多
基金supported by the Zhejiang Provincial Natural Science Foundation of China(LY23B060006 and LY18B060016).
文摘SAPO-5 zeolite supported RuMn was a highly efficient catalyst for the aqueous-phase selective hydrodeoxygenation of guaiacol to cyclohexanol.The optimal catalyst achieved a high cyclohexanol yield of 93.7%at full guaiacol conversion under mild conditions,with a high TOF of 920 h^(-1).Moreover,the catalyst displayed remarkable performance for the hydrogenation of phenol to cyclohexanol,where a 100%yield of cyclohexanol was obtained at a phenol-to-Ru molar ratio of about 17900.In particular,the catalyst exhibited excellent recyclability and could be recycled for 20 times without obvious activity loss.The as-prepared RuMn/SAPO-5 catalyst exhibited higher performance than most of the reported Rubased catalysts.
基金the support from the National Natural Science Foundation of China(21838011)。
文摘Rational design of Zn-containing HZSM-5 zeolite(Zn/HZSM-5)with high reactivity and excellent aromatization performance for olefin aromatization is crucially desired.We develop a new and uncomplicated method to synthesize Zn/HZSM-5(IMX/Z5)with superior aromatization performance in the paper.Compared to incipient wetness impregnation(IMP/Z5)and mechanical mixing(MIX/Z5),the asprepared IMX/Z5 presents a higher amount of surface ZnOH^(+)species(2.87%)while keeping identical bulk zinc content.As a result,more surface ZnOH^(+)favor both the aromatization of 1-hexene and cyclohexane dehydrogenation.For the two olefin aromatization pathways(hydrogen transfer and dehydrogenation),it is the first time found both the hydrogen transfer ability and the dehydrogenation ability increase linearly with the amount of surface ZnOH^(+)species while keeping identical bulk zinc content.We believe that the linear relationships are essential to design next generation olefin aromatization catalysts.
基金National Natural Science Foundation of China(No.21908085,21776129,and 21706121)Natural Science Foundation of Jiangsu Province(No.BK20170995 and BK20190961)+1 种基金General Program for University Natural Science Research of Jiangsu Province(No.16KJB530003)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘The oxidative desulphurization(ODS)has become mainly popular by rapid catalytic oxidation of dibenzothiophene(DBT)relied on efficient heterogeneous catalyst,V-based catalytic active species were regarded as the potential option in the activity-preferred ODS systems.Herein,we reported the redispersion of vanadium oxide(VO_(χ))on the mesoporous silica modified with manganese oxide(Mn_(3)O_(4)) through one progressive insertion approach of metal oxides in the silica.Impressively,mesoporeencaged vanadium-manganese oxides in the silica(VMn-MS)as the admirable output of excellent ODS catalyst was demonstrated compared to other monometal-modified counterparts and one-pot implanted one.The characterization results revealed the post-implanted VO_(χ) species not only deposited around the pre-covered Mn_(3)O_(4) on the mesoporous surface but also inserted the surface layer of Mn_(3)O_(4) inducing the amorphous evolution of aggregated Mn_(3)O_(4) and the reconstruction of final active sites.This integrated approach made the reconstructed active species afford more exposed catalytic sites and the tailored surface redox cycles owing to the electronic communication of V-Mn.The catalytic results demonstrated the excellent catalytic desulphurization efficiency(~100%)during 60 min at 80℃,which made the sulphur content reduce to 6 mg·L^(-1),remarkably superior to other comparative samples.The outstanding catalytic performance of VMn-MS catalyst can be ascribed to the synergistic effect of V-Mn dual metals rendering two different reaction pathways,which includes free-radical reaction and ring-forming reaction,where Mn site acted as active center triggering reactive free radicals which could be further optimized by surrounded V sites around Mn sites to promote the ODS process.
文摘目的探讨经门静脉胰岛细胞移植(PIT)后,细胞间粘附分子-1(ICAM-1)的表达与移植免疫排斥反应的关系,为胰岛细胞移植术后排斥反应的临床治疗提供理论依据。方法30只Wistar糖尿病大鼠随机分为三组,A组:糖尿病模型组(n=10),不做任何处理;B组:生理盐水组(n=10),采用腹腔注射生理盐水2ml/d;C组:免疫抑制剂组(n=10),采用腹腔注射CsA(3mg·kg^-1.d^-1)+MMF(20mg·kg^-1.d^-1);全部采取SD大鼠胰岛细胞→Wistar大鼠糖尿病动物模型。观察:①各组胰岛细胞移植术后第1、4、7、10、30、60天大鼠外周血血糖的变化;②流式细胞仪(Elite Coulter Company US)技术检测胰岛细胞移植术后外周血粘附分子ICAM-1的表达情况;③免疫组化方法检测各组胰岛细胞移植术后第10、60天,肝脏中ICAM-1的表达水平。结果①血糖值变化:术前各组间血糖值比较无统计学差异(P=0.669);B、C组血糖在术后第7或10天达最低水平,之后逐渐上升;任何两组间比较有统计学差异。②外周血ICAM-1的表达情况:术前各组间ICAM-1值比较无统计学差异(P=0.754);术后C组在第7或10天达最低水平,以后逐渐上升,最后接近B组水平;任何两组间比较有统计学差异。③肝脏粘附分子表达:术后10d和术后60d比较:A组(P=0.816)无统计学差异,B组(P=0.855)无统计学差异,C组(P=0.000)有统计学差异;术后10d:任何两组间均存在统计学差异(P<0.05);术后60d:B组与C组无统计学差异,A组同任何组均存在统计学差异(P<0.05)。结论PIT后粘附分子的变化与免疫排斥反应的发生有很大的相关性,进而和移植物功能有一定的相关性,且粘附分子表达水平的升高可以预示免疫排斥反应的发生。
