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
Mg-Al hydrotalcites were synthesized using different preparation methods(a co-precipitation method, a urea method, and a simple one) to analyze their effect on the catalytic activity of these solid base catalysts. The...Mg-Al hydrotalcites were synthesized using different preparation methods(a co-precipitation method, a urea method, and a simple one) to analyze their effect on the catalytic activity of these solid base catalysts. The method strongly affected the structure of their layers(e.g., the growth and stacking of the layers, and the type of intercalated anions) and, accordingly, their catalytic activity. The Mg-Al hydrotalcite prepared by co-precipitation showed the best catalytic performance in the isomerization of glucose into fructose, due to the small crystallite size and sand rose morphology enhancing the exposure of surface active sites to reactants.展开更多
Mg/Al/Fe layered double hydroxide(MAF-LDH1) was prepared by solvothermal method with the sodium dodecyl sulfate as the template, and the ethanol system was benefit to growth of sample. The nature in the resulting MAF-...Mg/Al/Fe layered double hydroxide(MAF-LDH1) was prepared by solvothermal method with the sodium dodecyl sulfate as the template, and the ethanol system was benefit to growth of sample. The nature in the resulting MAF-LDH was investigated by X-ray diffraction, field emission scanning electron microscopy, Fourier transformed infrared spectra, thermogravimetric analysis, and N2 adsorption-desorption.The morphology of MAF-LDH1 is petal-like with the size of 400-500 nm and the thickness about 10-20 nm. The adsorption performance of the samples was evaluated by absorption of the Congo red(CR) solutions. Compared with Mg/Al layered double hydroxide(MA-LDH), the maximum adsorption capacities of the MAF-LDH1 samples were 943.4 mg/g which was greatly enhanced. Furthermore, after seven cycling tests, the adsorption performance was still up to 90%. Theoretical calculation results revealed that the adsorption process was spontaneous and followed the pseudo-second-order kinetic model and Freundlich model. This work provides a promising alternative strategy to enhance the adsorptive properties of hydrotalcite-like materials.展开更多
Trace amounts of noble metal-doped Ni/Mg（AI）O catalysts were pre- pared starting from Mg-Al hydrotalcites （HTs） and tested in daily start-up and shut-down （DSS） operation of steam reforming （SR） of methane or ...Trace amounts of noble metal-doped Ni/Mg（AI）O catalysts were pre- pared starting from Mg-Al hydrotalcites （HTs） and tested in daily start-up and shut-down （DSS） operation of steam reforming （SR） of methane or partial oxidation （PO） of propane. Although Ni/Mg（Al）O catalysts prepared from Mg（Ni）-Al HT exhibited high and stable activity in stationary SR, PO and dry reforming of methane and propane, the Ni/Mg（Al）O catalysts were drastically deactivated due to Ni oxidation by steam as purge gas when they were applied in DSS SR of methane. Such deactivation was effectively suppressed by doping trace amounts of noble metal on the catalysts by using a ＂memory effect＂ of HTs. Moreover, the noble metal-doped Ni/Mg（Al）O catalysts exhibited ＂intelligent＂ catalytic behaviors, i.e., self-activation and self-regenerative activity, leading to high and sustainable activity during DSS operation. Pt was the most effective among noble metals tested. The self-activation occurred by the reduction of Ni2＋ in Mg（Ni,Al）O periclase to Ni^0 assisted by hydrogen spillover from Pt （or Pt-Ni alloy）. The self-regenerative activity was accomplished by self-redispersion of active Ni^0 particles due to a reversible reductionoxidation movement of Ni between the outside and the inside of the Mg（Al）O periclase crystal; surface Ni^0 was oxidized to Ni2＋ by steam and incorporated into Mg（Ni2＋,Al）O periclase, whereas the Ni2＋ in the periclase was reduced to Ni^0 by the hydrogen spillover and appeared as the fine Ni^0 particles on the catalyst surface. Further a ＂green＂ preparation of the Pt/Ni/[Mg3.sAl]O catalysts was accomplished starting from commercial Mg3.5-AI HT by calcination, followed by sequential impregnation of Ni and Pt.展开更多
Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was inves...Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was investigated with dry reforming of methane.Experimental results showed that the hydrotalcite-like precursors could be completely decomposed and partly reduced by cold plasma jet,and the Nicontained catalysts exhibited much higher activity than the catalyst without Ni.Especially,the catalyst with Ni/Co ratio of 8/2 achieved not only the highest conversions of 80.3%and 69.3%for CH4 and CO2,respectively,but also the best stability in 100 h testing.The catalysts were characterized by XRD,XPS,TEM and N2 adsorption techniques,and the results showed that the better performance of the 8Ni2Co bimetallic catalyst was attributed to its higher metal dispersion,smaller metal particle size,as well as the interaction effect between Ni and Co,which were brought by the special catalyst preparation method.展开更多
To study the modification mechanism of activated carbon(AC)by Fe and the low-temperature NH_(3)-selective catalytic reduction(SCR)denitration mechanism of Fe/AC catalysts,Fe/AC catalysts were prepared using coconut sh...To study the modification mechanism of activated carbon(AC)by Fe and the low-temperature NH_(3)-selective catalytic reduction(SCR)denitration mechanism of Fe/AC catalysts,Fe/AC catalysts were prepared using coconut shell AC activated by nitric acid as the support and iron oxide as the active component.The crystal structure,surface morphology,pore structure,functional groups and valence states of the active components of Fe/AC catalysts were characterised by X-ray diffraction,scanning electron microscopy,nitrogen adsorption and desorption,Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy,respectively.The effect of Fe loading and calcination temperature on the low-temperature denitration of NH_(3)-SCR over Fe/AC catalysts was studied using NH_(3)as the reducing gas at low temperature(150℃).The results show that the iron oxide on the Fe/AC catalyst is spherical and uniformly dispersed on the surface of AC,thereby improving the crystallisation performance and increasing the number of active sites and specific surface area on AC in contact with the reaction gas.Hence,a rapid NH_(3)-SCR reaction was realised.When the roasting temperature remains constant,the iron oxide crystals formed by increasing the amount of loading can enter the AC pore structure and accumulate to form more micropores.When the roasting temperature is raised from 400 to 500℃,the iron oxide is mainly transformed fromα-Fe_(2)O_(3)toγ-Fe_(2)O_(3),which improves the iron oxide dispersion and increases its denitration active site,allowing gas adsorption.When the Fe loading amount is 10%,and the roasting temperature is 500℃,the NO removal rate of the Fe/AC catalyst can reach 95%.According to the study,the low-temperature NH_(3)-SCR mechanism of Fe/AC catalyst is proposed,in which the redox reaction between Fe~(2+)and Fe~(3+)will facilitate the formation of reactive oxygen vacancies,which increases the amount of oxygen adsorption on the surface,especially the increase in surface acid sites,and promotes and adsorbs more reaction gases(NH_(3),O_(2),NO).The transformation from the standard SCR reaction to the fast SCR reaction is accelerated.展开更多
An efficient synthesis of benzoin isopropyl ether with benzaldehyde and propanol in the presence of heterogeneous recyclable Cu-Fe-hydrotalcite catalyst has been explored. Cu-Fe-hydrotalcite was firstly successfully s...An efficient synthesis of benzoin isopropyl ether with benzaldehyde and propanol in the presence of heterogeneous recyclable Cu-Fe-hydrotalcite catalyst has been explored. Cu-Fe-hydrotalcite was firstly successfully synthesized over Jahn-Teller effect of Cu^2＋. The catalytic test result showed that Cu-Fe-hydrotalcite could be used as a good catalyst in the synthesis of benzoin isopropyl ether. The highest conversion of ben- zaldehyde was 59.7% and the selectivity of benzoin isopropyl ether was nearly 100%. By this new method, not only was the cyanide poisoning avoided, but also the synthesis of benzoin isopropyl ether could be completed in one step instead of traditional two steps with both condensation and etherification.展开更多
The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,th...The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.展开更多
Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air bat...Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries.Although Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active sites.Motivated by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N precursors.Benefitting from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 h.Molecular dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C SAC-950.This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.展开更多
<p align="justify"> <span style="font-family:Verdana;">The review outcome represents the optimum catalytic conditions </span><span><span><span style="font-fami...<p align="justify"> <span style="font-family:Verdana;">The review outcome represents the optimum catalytic conditions </span><span><span><span style="font-family:'Minion Pro Capt','serif';"><span style="font-family:Verdana;">for the pro</span><span style="font-family:Verdana;">duction of hydrogen using hydrotalcite derived catalysts. It covers dr</span><span style="font-family:Verdana;">y and ste</span><span style="font-family:Verdana;">am reforming of methane, steam reforming of methanol and ethanol t</span><span style="font-family:Verdana;">o hydrogen. The review also revealed the specific properties of hydrotalcite der</span><span style="font-family:Verdana;">ived catalysts for the reactions. Among catalyst investigated, Ni & Fe</span><span style="font-family:Verdana;"> promoted Al-Mg containing hydrotalcite catalyst perform best (99%) for dry reforming of methane at 250°C. For steam methane reforming, Ni containing </span><span style="font-family:Verdana;">ca-aluminates hydrotalcite catalyst act as the best (99%) at 550°C. Cu-supporte</span><span style="font-family:Verdana;">d Zn-Al-containing catalyst performs the best (99.98%) for steam reforming of methanol at 300°C whereas Cu impregnated Mg-Al containing hydrotalcite is </span><span style="font-family:Verdana;">the best (99%) for steam reforming of ethanol at 200°C - 600°C. It’s (HT</span><span style="font-family:Verdana;">) tunable and versatile textural and morphological properties showed excellent catalytic performances for different industrial processes and in sustainable hydrogen production.</span></span></span></span> </p>展开更多
Poly(ethylene terephthalate)(PET)was synthesized by the in-situ polymerization method using layered double hydrotalcite(LDH)as the catalyst,and the thermal and flame retardation properties of PET were investigated as ...Poly(ethylene terephthalate)(PET)was synthesized by the in-situ polymerization method using layered double hydrotalcite(LDH)as the catalyst,and the thermal and flame retardation properties of PET were investigated as required.As identified by differential scanning calorimetry(DSC)and thermogravimetric(TGA)analysis,the crystallization rate and thermal degradation temperature of the as-prepared PET sample were enhanced compared with commercial PET sample.It was confirmed from the fire-resistant property study that the LDH can be used as an efficient flame-retardant besides functioning as a catalyst in the transesterification/polycondensation process for PET synthesis.展开更多
Fe（HSO4）3 has been used as an efficient and recyclable catalyst for the one-pot synthesis of 14-aryl- or alkyl-14Hdibenzo[aj]xanthene derivatives by the reaction of 2-naphtol and aldehydes. Different types of aromat...Fe（HSO4）3 has been used as an efficient and recyclable catalyst for the one-pot synthesis of 14-aryl- or alkyl-14Hdibenzo[aj]xanthene derivatives by the reaction of 2-naphtol and aldehydes. Different types of aromatic and aliphatic aldehydes are used in the reaction and in all cases the products were obtained in good to excellent yields.展开更多
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.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea funded by the Ministry of Education (NRF-2015R1D1A1A01059724)
文摘Mg-Al hydrotalcites were synthesized using different preparation methods(a co-precipitation method, a urea method, and a simple one) to analyze their effect on the catalytic activity of these solid base catalysts. The method strongly affected the structure of their layers(e.g., the growth and stacking of the layers, and the type of intercalated anions) and, accordingly, their catalytic activity. The Mg-Al hydrotalcite prepared by co-precipitation showed the best catalytic performance in the isomerization of glucose into fructose, due to the small crystallite size and sand rose morphology enhancing the exposure of surface active sites to reactants.
基金Funded by the Science and Technology Development Plan Project of Shandong Province,China(No.2013GSF11714)the Open Project of Hunan Sustentation Fund:Key Laboratory of Applied Environmental Photocatalysis,China(No.ccsu-KF-1501)
文摘Mg/Al/Fe layered double hydroxide(MAF-LDH1) was prepared by solvothermal method with the sodium dodecyl sulfate as the template, and the ethanol system was benefit to growth of sample. The nature in the resulting MAF-LDH was investigated by X-ray diffraction, field emission scanning electron microscopy, Fourier transformed infrared spectra, thermogravimetric analysis, and N2 adsorption-desorption.The morphology of MAF-LDH1 is petal-like with the size of 400-500 nm and the thickness about 10-20 nm. The adsorption performance of the samples was evaluated by absorption of the Congo red(CR) solutions. Compared with Mg/Al layered double hydroxide(MA-LDH), the maximum adsorption capacities of the MAF-LDH1 samples were 943.4 mg/g which was greatly enhanced. Furthermore, after seven cycling tests, the adsorption performance was still up to 90%. Theoretical calculation results revealed that the adsorption process was spontaneous and followed the pseudo-second-order kinetic model and Freundlich model. This work provides a promising alternative strategy to enhance the adsorptive properties of hydrotalcite-like materials.
基金supported by the New Energy and Industrial Technology Development Organization (NEDO),Japan
文摘Trace amounts of noble metal-doped Ni/Mg（AI）O catalysts were pre- pared starting from Mg-Al hydrotalcites （HTs） and tested in daily start-up and shut-down （DSS） operation of steam reforming （SR） of methane or partial oxidation （PO） of propane. Although Ni/Mg（Al）O catalysts prepared from Mg（Ni）-Al HT exhibited high and stable activity in stationary SR, PO and dry reforming of methane and propane, the Ni/Mg（Al）O catalysts were drastically deactivated due to Ni oxidation by steam as purge gas when they were applied in DSS SR of methane. Such deactivation was effectively suppressed by doping trace amounts of noble metal on the catalysts by using a ＂memory effect＂ of HTs. Moreover, the noble metal-doped Ni/Mg（Al）O catalysts exhibited ＂intelligent＂ catalytic behaviors, i.e., self-activation and self-regenerative activity, leading to high and sustainable activity during DSS operation. Pt was the most effective among noble metals tested. The self-activation occurred by the reduction of Ni2＋ in Mg（Ni,Al）O periclase to Ni^0 assisted by hydrogen spillover from Pt （or Pt-Ni alloy）. The self-regenerative activity was accomplished by self-redispersion of active Ni^0 particles due to a reversible reductionoxidation movement of Ni between the outside and the inside of the Mg（Al）O periclase crystal; surface Ni^0 was oxidized to Ni2＋ by steam and incorporated into Mg（Ni2＋,Al）O periclase, whereas the Ni2＋ in the periclase was reduced to Ni^0 by the hydrogen spillover and appeared as the fine Ni^0 particles on the catalyst surface. Further a ＂green＂ preparation of the Pt/Ni/[Mg3.sAl]O catalysts was accomplished starting from commercial Mg3.5-AI HT by calcination, followed by sequential impregnation of Ni and Pt.
基金supported by the National Natural Science Foundation of China(11075113)
文摘Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was investigated with dry reforming of methane.Experimental results showed that the hydrotalcite-like precursors could be completely decomposed and partly reduced by cold plasma jet,and the Nicontained catalysts exhibited much higher activity than the catalyst without Ni.Especially,the catalyst with Ni/Co ratio of 8/2 achieved not only the highest conversions of 80.3%and 69.3%for CH4 and CO2,respectively,but also the best stability in 100 h testing.The catalysts were characterized by XRD,XPS,TEM and N2 adsorption techniques,and the results showed that the better performance of the 8Ni2Co bimetallic catalyst was attributed to its higher metal dispersion,smaller metal particle size,as well as the interaction effect between Ni and Co,which were brought by the special catalyst preparation method.
基金Funded by the General Project of Science and Technology Plan of Yunnan Science and Technology Department(Nos.202001AT070029,2019FB077)Open Fund of Key Laboratory for Ferrous Metallurgy and Resources Utilization of Ministry of Education(No.FMRUlab-20-4)。
文摘To study the modification mechanism of activated carbon(AC)by Fe and the low-temperature NH_(3)-selective catalytic reduction(SCR)denitration mechanism of Fe/AC catalysts,Fe/AC catalysts were prepared using coconut shell AC activated by nitric acid as the support and iron oxide as the active component.The crystal structure,surface morphology,pore structure,functional groups and valence states of the active components of Fe/AC catalysts were characterised by X-ray diffraction,scanning electron microscopy,nitrogen adsorption and desorption,Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy,respectively.The effect of Fe loading and calcination temperature on the low-temperature denitration of NH_(3)-SCR over Fe/AC catalysts was studied using NH_(3)as the reducing gas at low temperature(150℃).The results show that the iron oxide on the Fe/AC catalyst is spherical and uniformly dispersed on the surface of AC,thereby improving the crystallisation performance and increasing the number of active sites and specific surface area on AC in contact with the reaction gas.Hence,a rapid NH_(3)-SCR reaction was realised.When the roasting temperature remains constant,the iron oxide crystals formed by increasing the amount of loading can enter the AC pore structure and accumulate to form more micropores.When the roasting temperature is raised from 400 to 500℃,the iron oxide is mainly transformed fromα-Fe_(2)O_(3)toγ-Fe_(2)O_(3),which improves the iron oxide dispersion and increases its denitration active site,allowing gas adsorption.When the Fe loading amount is 10%,and the roasting temperature is 500℃,the NO removal rate of the Fe/AC catalyst can reach 95%.According to the study,the low-temperature NH_(3)-SCR mechanism of Fe/AC catalyst is proposed,in which the redox reaction between Fe~(2+)and Fe~(3+)will facilitate the formation of reactive oxygen vacancies,which increases the amount of oxygen adsorption on the surface,especially the increase in surface acid sites,and promotes and adsorbs more reaction gases(NH_(3),O_(2),NO).The transformation from the standard SCR reaction to the fast SCR reaction is accelerated.
基金support from the National Natural Science Foundation of China (50872086)the Natural Science Foundation of Shanxi Province(2008011018)
文摘An efficient synthesis of benzoin isopropyl ether with benzaldehyde and propanol in the presence of heterogeneous recyclable Cu-Fe-hydrotalcite catalyst has been explored. Cu-Fe-hydrotalcite was firstly successfully synthesized over Jahn-Teller effect of Cu^2＋. The catalytic test result showed that Cu-Fe-hydrotalcite could be used as a good catalyst in the synthesis of benzoin isopropyl ether. The highest conversion of ben- zaldehyde was 59.7% and the selectivity of benzoin isopropyl ether was nearly 100%. By this new method, not only was the cyanide poisoning avoided, but also the synthesis of benzoin isopropyl ether could be completed in one step instead of traditional two steps with both condensation and etherification.
基金gratefully acknowledge the financial support of the National Natural Science Foundation of China(22108145 and 21978143)the Shandong Province Natural Science Foundation(ZR2020QB189)+1 种基金State Key Laboratory of Heavy Oil Processing(SKLHOP202203008)the Talent Foundation funded by Province and Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering(STHGYX2201).
文摘The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.
基金financially supported by the National Key R&D Program of China(2022YFB4004100)the National Natural Science Foundation of China(22272161)+6 种基金the Jilin Province Science and Technology Development Program(20230101367JC)financially supported by the National Natural Science Foundation of China(22073094)the Science and Technology Development Program of Jilin Province(20210402059GH)the Science and Technology Plan Projects of Yunnan Province(202101BC070001–007)the Major Science and Technology Projects for Independent Innovation of China FAW Group Co.,Ltd(20220301018GX)the essential support of the Network and Computing Center,CIAC,CASthe Computing Center of Jilin Province。
文摘Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries.Although Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active sites.Motivated by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N precursors.Benefitting from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 h.Molecular dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C SAC-950.This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.
文摘<p align="justify"> <span style="font-family:Verdana;">The review outcome represents the optimum catalytic conditions </span><span><span><span style="font-family:'Minion Pro Capt','serif';"><span style="font-family:Verdana;">for the pro</span><span style="font-family:Verdana;">duction of hydrogen using hydrotalcite derived catalysts. It covers dr</span><span style="font-family:Verdana;">y and ste</span><span style="font-family:Verdana;">am reforming of methane, steam reforming of methanol and ethanol t</span><span style="font-family:Verdana;">o hydrogen. The review also revealed the specific properties of hydrotalcite der</span><span style="font-family:Verdana;">ived catalysts for the reactions. Among catalyst investigated, Ni & Fe</span><span style="font-family:Verdana;"> promoted Al-Mg containing hydrotalcite catalyst perform best (99%) for dry reforming of methane at 250°C. For steam methane reforming, Ni containing </span><span style="font-family:Verdana;">ca-aluminates hydrotalcite catalyst act as the best (99%) at 550°C. Cu-supporte</span><span style="font-family:Verdana;">d Zn-Al-containing catalyst performs the best (99.98%) for steam reforming of methanol at 300°C whereas Cu impregnated Mg-Al containing hydrotalcite is </span><span style="font-family:Verdana;">the best (99%) for steam reforming of ethanol at 200°C - 600°C. It’s (HT</span><span style="font-family:Verdana;">) tunable and versatile textural and morphological properties showed excellent catalytic performances for different industrial processes and in sustainable hydrogen production.</span></span></span></span> </p>
文摘Poly(ethylene terephthalate)(PET)was synthesized by the in-situ polymerization method using layered double hydrotalcite(LDH)as the catalyst,and the thermal and flame retardation properties of PET were investigated as required.As identified by differential scanning calorimetry(DSC)and thermogravimetric(TGA)analysis,the crystallization rate and thermal degradation temperature of the as-prepared PET sample were enhanced compared with commercial PET sample.It was confirmed from the fire-resistant property study that the LDH can be used as an efficient flame-retardant besides functioning as a catalyst in the transesterification/polycondensation process for PET synthesis.
文摘Fe（HSO4）3 has been used as an efficient and recyclable catalyst for the one-pot synthesis of 14-aryl- or alkyl-14Hdibenzo[aj]xanthene derivatives by the reaction of 2-naphtol and aldehydes. Different types of aromatic and aliphatic aldehydes are used in the reaction and in all cases the products were obtained in good to excellent yields.
