In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a pro...In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock.This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels.Following a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively discussed.Either in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino acids.On the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive compounds.The review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging strategies.Finally,opportunities,challenges and prospective of woody biomass valorization are highlighted.展开更多
The adsorptive separation of C_(2)H_(4)and C_(2)H_(6),as an alternative to distillation units consuming high energy,is a promising yet challenging research.The great similarity in the molecular size of C_(2)H_(4)and C...The adsorptive separation of C_(2)H_(4)and C_(2)H_(6),as an alternative to distillation units consuming high energy,is a promising yet challenging research.The great similarity in the molecular size of C_(2)H_(4)and C_(2)H_(6)brings challenges to the regulation of adsorbents to realize efficient dynamic separation.Herein,we reported the enhancement of the kinetic separation of C_(2)H_(4)/C_(2)H_(6)by controlling the crystal size of ZnAtzPO_(4)(Atz=3-amino-1,2,4-triazole)to amplify the diffusion difference of C_(2)H_(4)and C_(2)H_(6).Through adjusting the synthesis temperature,reactant concentration,and ligands/metal ions molar ratio,ZnAtzPO4 crystals with different sizes were obtained.Both single-component kinetic adsorption tests and binary-component dynamic breakthrough experiments confirmed the enhancement of the dynamic separation of C_(2)H_(4)/C_(2)H_(6)with the increase in the crystal size of ZnAtzPO_(4).The separation selectivity of C_(2)H_(4)/C_(2)H_(6)increased from 1.3 to 98.5 with the increase in the crystal size of ZnAtzPO_(4).This work demonstrated the role of morphology and size control of adsorbent crystals in the improvement of the C_(2)H_(4)/C_(2)H_(6)kinetic separation performance.展开更多
Compared to inorganic supports, polymeric supports can offer additional benefits, e.g., easier processing and cheaper. However, the organic surface has weak adhesion to the zeolitic imidazolate frameworks(ZIFs) membra...Compared to inorganic supports, polymeric supports can offer additional benefits, e.g., easier processing and cheaper. However, the organic surface has weak adhesion to the zeolitic imidazolate frameworks(ZIFs) membrane layer, which usually requires complex surface modification or seeding. Herein, we demonstrate that a dual-layer asymmetric polymer support prepared by a simple spinning process is a good candidate for the preparation of ZIF-8 membrane. The inner layer of the support is an organic hollow fiber(PES) with finger-like pores, and the outer layer is a ZnO-PES composite layer with finger-like pores also. The ZnO-PES composite layer is expected to contain uniform ZnO crystals in the polymer matrix, i.e., the ZnO particles in the skin layer of the support are not easy to fall off. Under the induction of ZnO particles in the outer layers, continuous ZIF-8 membranes can be prepared by single in-situ crystallization, showing good adhesion to the supports. The obtained ZIF-8 membranes show a H_(2) permeance of 8.7 × 10^(-8)mol·m^(-2)·s^(-1)·Pa^(-1) with a H_(2)/N_(2) ideal separation selectivity of 18.0. The design and preparation of this dual-layer polymer support is expected to promote the large-scale application of MOF membranes on polymer supports.展开更多
Infectious bursal disease(IBD)causes considerable economic losses in the commercial poultry industry worldwide.The principal way to control IBD virus(IBDV),the causative agent of IBD,is still through vaccination progr...Infectious bursal disease(IBD)causes considerable economic losses in the commercial poultry industry worldwide.The principal way to control IBD virus(IBDV),the causative agent of IBD,is still through vaccination programs.Virus-like particles(VLPs)are recognised as a safe and potent recombinant vaccine platform.This research work explores the characterisation and separation of infectious bursal disease virus-like particles(IBD-VLPs)from crude feedstock.Various characteristics were studied with highperformance size-exclusion chromatography(HP-SEC),sodium dodecyl sulphate–polyacrylamide gel electrophoresis(SDS-PAGE)and transmission electron microscopy(TEM)analyses.Subsequently,the separation of IBD-VLPs using polyethylene glycol(PEG)/sodium citrate-based aqueous two-phase systems(ATPSs)was conducted and optimised.Moreover,a scale-up study of the best ATPS constituted of 15%PEG 6000,11%sodium citrate and 10%crude feedstock was performed to compare the separation performance of IBD-VLPs with and without centrifugation-assisted.The results indicated that the optimised ATPS with centrifugation-assisted for both 5 g and 50 g systems showed good recovery of IBDVLPs of>97%in the interphase between the PEG-rich top and salt-rich bottom phases.These optimised systems also showed high removal efficiencies of impurities of>95%.The results demonstrated that aqueous two-phase extraction could be a promising technology for efficient VLPs separation.展开更多
Gold catalysts supported on Mg-Al mixed oxides for oxidative esterification of methacrolein are prepared by impregnation.Effects of the support particle size,concentration of HAuCl4 solution and Mg/Al ratio on gold lo...Gold catalysts supported on Mg-Al mixed oxides for oxidative esterification of methacrolein are prepared by impregnation.Effects of the support particle size,concentration of HAuCl4 solution and Mg/Al ratio on gold loading and catalytic properties are investigated.The catalysts are characterized by CO_(2)-TPD,EDS,XPS,STEM and XRD techniques.Catalysts with smaller support particle size show more uniform gold distribution and higher gold dispersion,resulting in a higher catalytic performance,and the uniformity of gold and the activity of the catalysts with larger support particle size can be improved by decreasing the concentration of HAuCl4 solution.The Mg/Al molar ratio has significant effect on the uniformity of gold and the activity of the catalyst,and the optimum Mg/Al molar ratio is 0.1–0.2.This study underlines the importance of engineering support particle size,concentration of HAuCl4 solution and density of adsorption sites for efficient gold loading on support by impregnation.展开更多
Hydrodeoxygenation of furfural(FF)into 2-methylfuran(MF)is a significant biomass utilization route.However,designing efficient and stable non-noble metal catalyst is still a huge challenge.Herein,we reported the N,O c...Hydrodeoxygenation of furfural(FF)into 2-methylfuran(MF)is a significant biomass utilization route.However,designing efficient and stable non-noble metal catalyst is still a huge challenge.Herein,we reported the N,O co-doped carbon anchored with Co nanoparticles(Co-SFB)synthesized by employing the organic ligands with the target heteroatoms.Raman,electron paramagnetic resonance(EPR),electrochemical impedance spectroscopy(EIS),and X-ray photoelectron spectroscopy(XPS)characterizations showed that the co-doping of N and O heteroatoms in the carbon support endows Co-SFB with enriched lone pair electrons,fast electron transfer ability,and strong metal-support interaction.These electronic properties resulted in strong FF adsorption as well as lower apparent reaction activation energy.At last,the obtained N,O co-doped Co/C catalyst showed excellent catalytic activity(nearly 100 mol%FF conversion and 94.6 mol%MF yield)and stability for in-situ dehydrogenation of FF into MF.This N,O co-doping strategy for the synthesis of highly efficient catalytic materials with controllable electronic state will provide an excellent opportunity to better understand the structure-function relationship.展开更多
As a renewable biomass-based compound with wide applications in food additives,fine chemical synthesis and fuels,γ-valerolactone(GVL)has attached much attention.While,pyrrolidones are widely used in pharmaceutical,ag...As a renewable biomass-based compound with wide applications in food additives,fine chemical synthesis and fuels,γ-valerolactone(GVL)has attached much attention.While,pyrrolidones are widely used in pharmaceutical,agrochemical,material industrial and other chemical production.In this research,we demonstrated transformations of biomass-based ethyl levulinate(EL)into GVL and pyrrolidones by using heterogeneous catalysts(CNT-Ru-1)with N-heterocyclic carbene ruthenium(NHC-Ru)complex grafted on multi-walled carbon nanotube(CNT).The Ru catalyst showed high efficiency on EL hydrogenation to GVL with both EL conversion and GVL yield exceeding 99%.Moreover,the Ru catalyst readily promoted reductive amination of EL in the presence of various amines for pyrrolidone synthesis.Finally,the Ru catalyst was also applicable to hydrogenation of various carbonyl compounds for the synthesis of the corresponding alcohols with excellent catalytic performance.The research provides insight for heterogenizing the homogeneous noble metal-based catalysts with high catalytic active for biomass-based transformations.展开更多
The plasmonic photocatalyst of Pd supported on graphitic carbon nitride(Pd/g-C3N4)exhibits excellent catalytic activity in photo-induced hydrogenation of biomass-based aldehydes with environmental benign reagents of f...The plasmonic photocatalyst of Pd supported on graphitic carbon nitride(Pd/g-C3N4)exhibits excellent catalytic activity in photo-induced hydrogenation of biomass-based aldehydes with environmental benign reagents of formic acid(HCOOH)as proton source and triethylamine(TEA)as sacrificial electron donator.The chemical and configurational properties of the Pd/g-C3N4 were systematically analyzed with XRD,TEM and XPS.Under optimized conditions,27%yield of furfuryl alcohol with the corresponding turnover frequency(TOF)around 3.72 h^(-1) were obtained from furfural and TEA-HCOOH under visible-light irradiation by using Pd/g-C3N4.Our research additionally reveals that Pd atom is the true catalytic active site for the hydrogenation and the photo-promoted reduction mainly occurs through noble metal nanoparticles(NPs)-induced effect of surface plasmon resonance(SPR).The photo-catalytic system of Pd/g-C3N4 thus demonstrates a green and effective method for the hydrogenation of biomass-based aldehydes with sustainable solar energy as a driven force.展开更多
Pestalotiopsis sp. J63, producing a high activity of laccase, is a new marine-derived fungus isolated from the oceanic sediment of the East China Sea. Since the marine environment is oligotrophic nutrient, marine deri...Pestalotiopsis sp. J63, producing a high activity of laccase, is a new marine-derived fungus isolated from the oceanic sediment of the East China Sea. Since the marine environment is oligotrophic nutrient, marine derived fungi may use small amount of nutrients to grow and produce laccases. Agricultural residues that are mainly composed of lignin, cellulose and hemicellulose are difficult to be degraded and few microbes can take them as substrates, so they are considered as oligotrophic nutrient and have the potential to be used to produce value added products. In this study, the ability of Pestalotiopsis sp. J63 to use agricultural residues to produce laccases was tested in the submerged fermentation. The combination of 3 g·L 1maltose and 20 g·L 1rice straw was the best carbon sources and 8 g·L 1ammonium sulfate was the best nitrogen source under the condition without inducers. The effects of five inducers, the feeding time and concentration of inducer on laccase production were investigated.Adding 0.09 mmol·L 1phenol after 24 h of incubation led to high laccase activity(5089 U·L 1), while with 0.09mmol·L 1phenol in the medium and wheat bran as the nitrogen source, the laccase activity could reach 5791.7U·L 1. Native-PAGE results showed that two laccase isozymes were present in the cultures. One existed in both induced and non-induced culture filtrates, while the other was only found in the fermentation with the addition of phenol, guaiacol and veratryl alcohol.展开更多
Bioactive natural products are a main source of new drugs,functional foods and food additives.The separation of bioactive natural products plays an important role in transformation and use of biomass.The isolation and...Bioactive natural products are a main source of new drugs,functional foods and food additives.The separation of bioactive natural products plays an important role in transformation and use of biomass.The isolation and purification of bioactive principle from a complex matrix is often inherent bottleneck for the utilization of natural products,so a series of extraction and separation techniques have been developed.This review covers recent advances in the separation of bioactive natural products with an emphasis on their solubility and diffusion coefficients,recent extraction techniques and isolation techniques.This overview of recent technological advances,discussion of pertinent problems and prospect of current methodologies in the separation of bioactive natural products may provide a driving force for development of novel separation techniques.展开更多
To get deep understanding of the reaction mechanism of coal pyrolysis in hydrogen plasma, the decomposition reaction pathways of aliphatic hydrocarbons and cycloalkanes, which are two main components in volatiles from...To get deep understanding of the reaction mechanism of coal pyrolysis in hydrogen plasma, the decomposition reaction pathways of aliphatic hydrocarbons and cycloalkanes, which are two main components in volatiles from coal, were investigated. Methane and cyclohexane were chosen as the model compounds. Density functional theory was employed, and many reaction pathways were involved. Calculations were carried out in Gaussian 09 at the B3LYP/6-31G(d,p) level of the theory. The results indicate that the main pyrolysis products of methane and cyclohexane in hydrogen plasma are both hydrogen and acetylene, and the participation of active hydrogen atoms makes dehydrogenation reactions more favorable. H2 mainly comes from dehydrogenation process, while many reaction pathways are responsible for acetylene formation. During coal pyrolysis in hydrogen plasma, three main components in volatiles like aliphatic hydrocarbons, cycloalkanes and aromatic hydrocarbons lead to the formation of hydrogen and acetylene, but their contributions to products distribution are different.展开更多
In order to improve the efficient decolorization of dye-containing water by biosorbent and understand the biosorption mechanism, the self-immobilization mycelial pellets were prepared using a marine-derived fungus Asp...In order to improve the efficient decolorization of dye-containing water by biosorbent and understand the biosorption mechanism, the self-immobilization mycelial pellets were prepared using a marine-derived fungus Aspergillus niger ZJUBE-1, and an azo dye, Congo red was chosen as a model dye to investigate batch decolorization efficiency by pellets. The pellets as biosorbent showed strong salt and acid tolerance in biosorption process. The results for dye adsorption showed that the biosorption process fitted well with models of pseudo-second-order kinetic and Langmuir isotherm, with a maximum adsorption capacity of 263.2 mg·g^(-1) mycelium. During 6 batches of continuous decolorization operation, the mycelial pellets could possess efficient decolorization abilities(>98.5%).The appearance of new peak in the UV–Vis spectral result indicated that the decolorization process may also contain biodegradation. The mechanism studies showed that efficient biosorption ability of pellets only relies on the active zone on the surface of the pellet, which can be enhanced by nutrition supplement or be shifted outward by a reculture process.展开更多
Hydrogenation of carbazole and N-ethylcarbazole over Raney-Ni catalyst were realized in the temperature range of 393-503 K. 4[H] adduct dominated the hydrogenation products and the formation of 2[H] adduct was the rat...Hydrogenation of carbazole and N-ethylcarbazole over Raney-Ni catalyst were realized in the temperature range of 393-503 K. 4[H] adduct dominated the hydrogenation products and the formation of 2[H] adduct was the rate-limiting step during the period, in which the conversion of carbazole was less than 40%. The hydrogenation process followed pseudo-first-order kinetics and the hydrogenation activation energies of carbazole and N-ethylcarbazole were 90 k J/mol and 115 k J/mol, respectively. The reaction starting position as well as the pathway of the hydrogenation of(N-ethyl)carbazole were investigated by comparing the kinetic characteristics of hydrogen uptake of carbazole and Nethylcarbazole. The results showed that the reaction was a stepwise hydrogenation process and the first H2 was added to the C1 = C10 double bond in the hydrogenation.展开更多
Industrial grade multi-walled carbon nanotubes(IG-MWCNTs) are a low-cost substitute for commercially purified multi-walled carbon nanotubes(P-MWCNTs). In this work, IG-MWCNTs were functionalized with tetraethylenepent...Industrial grade multi-walled carbon nanotubes(IG-MWCNTs) are a low-cost substitute for commercially purified multi-walled carbon nanotubes(P-MWCNTs). In this work, IG-MWCNTs were functionalized with tetraethylenepentamine(TEPA) for CO2capture. The TEPA impregnated IG-MWCNTs were characterized with various experimental methods including N2adsorption/desorption isotherms, elemental analysis, X-ray diffraction, Fourier transform infrared spectroscopy and thermogravimetric analysis. Both the adsorption isotherms of IGMWCNTs-n and the isosteric heats of different adsorption capacities were obtained from experiments. TEPA impregnated IG-MWCNTs were also shown to have high CO2adsorption capacity comparable to that of TEPA impregnated P-MWCNTs. The adsorption capacity of IG-MWCNTs based adsorbents was in the range of 2.145 to 3.088 mmol/g, depending on adsorption temperatures. Having the advantages of low-cost and high adsorption capacity, TEPA impregnated IG-MWCNTs seem to be a promising adsorbent for CO2capture from flue gas.展开更多
This review intends to introduce the application of lignin-derived catalyst for green organic synthesis over latest two decades and aims to present a renewable alternative for conventional catalyst for future industry...This review intends to introduce the application of lignin-derived catalyst for green organic synthesis over latest two decades and aims to present a renewable alternative for conventional catalyst for future industry application. The structure of lignin is initially introduced in this review. Then, various pretreatment and activation technologies of lignin are systematically presented, which includes physical activation for the formation of well-developed porosity and chemical activation to introduce catalytic active sites. Finally, the catalytic performances of various lignin-derived catalysts are rationally assessed and compared with conventional catalysts, which involves lignin-derived solid acids for hydrolysis, hydration, dehydration(trans)esterification, multi-component reaction and condensation, lignin-derived solid base for Knoevenagel reaction, lignin-derived electro-catalysts for electro-oxidation, oxygen reduction reaction, and lignin-derived supported transition metal catalysts for hydrogenation, oxidation, coupling reaction, tandem reaction, condensation reaction, ring-opening reaction, Friedel-Crafts-type reaction,Fischer–Tropsch synthesis, click reaction, Glaser reaction, cycloaddition and(trans)esterification. The above lignin-derived catalysts thus successfully promote the transformations of organic compounds, carbon dioxide, biomass-based cellulose, saccharide and vegetable oil into valuable chemicals and fuels. At the end of this review, some perspectives are given on the current issues and tendency on the lignin-derived catalysts for green chemistry.展开更多
The sorption-enhanced steam reforming process of methanol(SESRP-Me OH) to produce high-purity H2 was thermodynamically and experimentally studied.Thermodynamic calculations showed that at a CO2 adsorption ratio of 95%...The sorption-enhanced steam reforming process of methanol(SESRP-Me OH) to produce high-purity H2 was thermodynamically and experimentally studied.Thermodynamic calculations showed that at a CO2 adsorption ratio of 95%,product gas contains 98.36% H2,32.8 ppm CO under temperature of 130°C and steam-to-methanol(S/M) molar ratio of 2.However,without adsorption-enhanced,the product gas contains nearly 74.99% H2 with 24.96% CO2 and 525 ppm CO.To verify the thermodynamic calculation results,experiments were performed in a fixed-bed reactor loaded with commercial Cu O/Zn O/Al2O3 methanol reforming catalyst and 22% K2CO3-promoted hydrotalcite as CO2 adsorbent.Experimental results showed that 99.61% H2 could be obtained by SESRP-Me OH at reaction temperature of 230°C and S/M of 2.Under the same CH3 OH conversion,the reaction temperature decreased by almost 50°C and H2 concentration increased of more than 20%using SESRP-Me OH compared with solely steam reforming of methanol.The characterization of the adsorbent and catalyst showed that the adsorbent showed good stability while the catalyst was seriously sintered under the high regeneration temperature of the adsorbent.展开更多
Five tryptophan analogues with a hydrophobic indole ring and an amino group on each molecule were used as functional ligands of mixed-mode resins for human serum albumin(HSA) purification. Their adsorption performance...Five tryptophan analogues with a hydrophobic indole ring and an amino group on each molecule were used as functional ligands of mixed-mode resins for human serum albumin(HSA) purification. Their adsorption performance was evaluated and the effects of p H and salt addition on HSA adsorption were studied. The resins prepared showed typical p H-dependent adsorption and the highest adsorption capacity and affinity were found at pH 5.0for all the resins tested. The saturated adsorption capacity was 138.02 mg·g^(-1)with the tryptaminefunctionalized resin, which significantly decreased at p H below 4.0 due to electrostatic repulsion between ligands and HSA. Moreover, the addition of Na Cl or(NH_4)_2SO_4in media reduced HSA adsorption capacity, although the two salts showed different affecting profiles. The tryptamine-functionalized resin showed the best salt-tolerant performance, and its high adsorption capacity was maintained under high salt concentrations. In addition, the five resins prepared showed good adsorption selectivity for recombinant HSA from Pichia pastoris broth. Molecular docking results between tryptamine and HSA indicated that tryptamine was favorable to bind on Site II(indole-binding site) of HSA.展开更多
Current–voltage(I–V) characteristics of hydrogen DC plasma torches with different sizes in an external axial magnetic field under atmospheric pressure are reported.Three anodes with different diameters are adopted i...Current–voltage(I–V) characteristics of hydrogen DC plasma torches with different sizes in an external axial magnetic field under atmospheric pressure are reported.Three anodes with different diameters are adopted in a 50-k W torch:25 mm,30 mm,and 35 mm,respectively.Two different diameters of anodes,that is,100 mm and 130 mm,are adopted in a 1-MW plasma torch.The arc voltage shows a negative trend with the increase of arc current under the operating regimes.On the contrary,arc voltage shows a positive trend as the flow rate of carrier gas increases,and a similar trend is found with increasing the external magnetic flux density.A similarity formula is constructed to correlate the experimental data of the torches mentioned above.Linear fitting shows that the Pearson correlation coefficient is 0.9958.展开更多
The importance of immunoglobulin Y(IgY) as a specific antibody equivalent to mammalian immunoglobulin G(IgG) is well recognized. However, production of highly purified IgY is still difficult due to the lack of specifi...The importance of immunoglobulin Y(IgY) as a specific antibody equivalent to mammalian immunoglobulin G(IgG) is well recognized. However, production of highly purified IgY is still difficult due to the lack of specific purification methods. In this study, adsorption behaviors of Ig Y on four mixed-mode resins with functional ligands of 4-mercatoethyl-pyridine(MEP), 2-mercapto-1-methyli-midazole(MMI), 5-aminobenzi-midazole(ABI) and tryptophan-5-aminobenzi-midazole(W-ABI) were evaluated. The results showed that high adsorption ratio were found at p H 6.0–7.0 with little adsorption under acidic conditions. The resin with ABI ligand was then used to separate IgY from immunized chicken serum. An efficient process with Ig Y purity of 95% and recovery of 90% was developed after optimization of loading and elution p H and injection volume. The biological activity of the purified Ig Y was fully maintained. These results indicated that mixed-mode chromatography with specially-designed ligands has great potential for the separation of Ig Y from crude feedstock.展开更多
Pulsed plasma discharge was employed to inactivate bacteria in the injection water for an oil field.The effects of water conductivity and initial concentration of bacteria on elimination efficiency were investigated i...Pulsed plasma discharge was employed to inactivate bacteria in the injection water for an oil field.The effects of water conductivity and initial concentration of bacteria on elimination efficiency were investigated in the batch and continuous flow modes.It was demonstrated that Fe^(2+) contained in injection water could enhance the elimination efficiency greatly.The addition of reducing agent glutathione(GSH) indicated that active radicals generated by pulsed plasma discharges played an important role in the inactivation of bacteria.Moreover,it was found that the microbial inactivation process for both batch and continuous flow mode well fitted the model based on the Weibull's survival function.展开更多
文摘In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock.This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels.Following a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively discussed.Either in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino acids.On the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive compounds.The review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging strategies.Finally,opportunities,challenges and prospective of woody biomass valorization are highlighted.
基金supported by the National Key Research and Development Program of China(2022YFB3806800)the National Natural Science Foundation of China(22122811,22008209)the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(2021SZ-TD008).
文摘The adsorptive separation of C_(2)H_(4)and C_(2)H_(6),as an alternative to distillation units consuming high energy,is a promising yet challenging research.The great similarity in the molecular size of C_(2)H_(4)and C_(2)H_(6)brings challenges to the regulation of adsorbents to realize efficient dynamic separation.Herein,we reported the enhancement of the kinetic separation of C_(2)H_(4)/C_(2)H_(6)by controlling the crystal size of ZnAtzPO_(4)(Atz=3-amino-1,2,4-triazole)to amplify the diffusion difference of C_(2)H_(4)and C_(2)H_(6).Through adjusting the synthesis temperature,reactant concentration,and ligands/metal ions molar ratio,ZnAtzPO4 crystals with different sizes were obtained.Both single-component kinetic adsorption tests and binary-component dynamic breakthrough experiments confirmed the enhancement of the dynamic separation of C_(2)H_(4)/C_(2)H_(6)with the increase in the crystal size of ZnAtzPO_(4).The separation selectivity of C_(2)H_(4)/C_(2)H_(6)increased from 1.3 to 98.5 with the increase in the crystal size of ZnAtzPO_(4).This work demonstrated the role of morphology and size control of adsorbent crystals in the improvement of the C_(2)H_(4)/C_(2)H_(6)kinetic separation performance.
基金supported by the National Natural Science Foundation of China (21978253)the Fundamental Research Funds for the Central Universities (226-2022-00020, 226-2022-00055)。
文摘Compared to inorganic supports, polymeric supports can offer additional benefits, e.g., easier processing and cheaper. However, the organic surface has weak adhesion to the zeolitic imidazolate frameworks(ZIFs) membrane layer, which usually requires complex surface modification or seeding. Herein, we demonstrate that a dual-layer asymmetric polymer support prepared by a simple spinning process is a good candidate for the preparation of ZIF-8 membrane. The inner layer of the support is an organic hollow fiber(PES) with finger-like pores, and the outer layer is a ZnO-PES composite layer with finger-like pores also. The ZnO-PES composite layer is expected to contain uniform ZnO crystals in the polymer matrix, i.e., the ZnO particles in the skin layer of the support are not easy to fall off. Under the induction of ZnO particles in the outer layers, continuous ZIF-8 membranes can be prepared by single in-situ crystallization, showing good adhesion to the supports. The obtained ZIF-8 membranes show a H_(2) permeance of 8.7 × 10^(-8)mol·m^(-2)·s^(-1)·Pa^(-1) with a H_(2)/N_(2) ideal separation selectivity of 18.0. The design and preparation of this dual-layer polymer support is expected to promote the large-scale application of MOF membranes on polymer supports.
基金Zhejiang University and TalentIntroduction Program of China for Postdoctoral Researcher for the financial supportfinancially supported by the National Key Research&Development Program of China (2021YFE0113300)the National Natural Science Foundation of China (22078286)。
文摘Infectious bursal disease(IBD)causes considerable economic losses in the commercial poultry industry worldwide.The principal way to control IBD virus(IBDV),the causative agent of IBD,is still through vaccination programs.Virus-like particles(VLPs)are recognised as a safe and potent recombinant vaccine platform.This research work explores the characterisation and separation of infectious bursal disease virus-like particles(IBD-VLPs)from crude feedstock.Various characteristics were studied with highperformance size-exclusion chromatography(HP-SEC),sodium dodecyl sulphate–polyacrylamide gel electrophoresis(SDS-PAGE)and transmission electron microscopy(TEM)analyses.Subsequently,the separation of IBD-VLPs using polyethylene glycol(PEG)/sodium citrate-based aqueous two-phase systems(ATPSs)was conducted and optimised.Moreover,a scale-up study of the best ATPS constituted of 15%PEG 6000,11%sodium citrate and 10%crude feedstock was performed to compare the separation performance of IBD-VLPs with and without centrifugation-assisted.The results indicated that the optimised ATPS with centrifugation-assisted for both 5 g and 50 g systems showed good recovery of IBDVLPs of>97%in the interphase between the PEG-rich top and salt-rich bottom phases.These optimised systems also showed high removal efficiencies of impurities of>95%.The results demonstrated that aqueous two-phase extraction could be a promising technology for efficient VLPs separation.
基金Open Project of Yunnan Precious Metals Laboratory Co.,Ltd(YPML-2023050269)the Fundamental Research Funds for the Central Universities(226-2023-00085,226-2023-00057).
文摘Gold catalysts supported on Mg-Al mixed oxides for oxidative esterification of methacrolein are prepared by impregnation.Effects of the support particle size,concentration of HAuCl4 solution and Mg/Al ratio on gold loading and catalytic properties are investigated.The catalysts are characterized by CO_(2)-TPD,EDS,XPS,STEM and XRD techniques.Catalysts with smaller support particle size show more uniform gold distribution and higher gold dispersion,resulting in a higher catalytic performance,and the uniformity of gold and the activity of the catalysts with larger support particle size can be improved by decreasing the concentration of HAuCl4 solution.The Mg/Al molar ratio has significant effect on the uniformity of gold and the activity of the catalyst,and the optimum Mg/Al molar ratio is 0.1–0.2.This study underlines the importance of engineering support particle size,concentration of HAuCl4 solution and density of adsorption sites for efficient gold loading on support by impregnation.
基金supported by the National Key R&D Program of China(2021YFC2103704)the National Natural Science Foundation of China(22022812,21978259)+1 种基金Key R&D Program of Zhejiang(2022C01208)Institute of Zhejiang University-Quzhou S&T Planed Projects(IZQ2021KJ1001)。
文摘Hydrodeoxygenation of furfural(FF)into 2-methylfuran(MF)is a significant biomass utilization route.However,designing efficient and stable non-noble metal catalyst is still a huge challenge.Herein,we reported the N,O co-doped carbon anchored with Co nanoparticles(Co-SFB)synthesized by employing the organic ligands with the target heteroatoms.Raman,electron paramagnetic resonance(EPR),electrochemical impedance spectroscopy(EIS),and X-ray photoelectron spectroscopy(XPS)characterizations showed that the co-doping of N and O heteroatoms in the carbon support endows Co-SFB with enriched lone pair electrons,fast electron transfer ability,and strong metal-support interaction.These electronic properties resulted in strong FF adsorption as well as lower apparent reaction activation energy.At last,the obtained N,O co-doped Co/C catalyst showed excellent catalytic activity(nearly 100 mol%FF conversion and 94.6 mol%MF yield)and stability for in-situ dehydrogenation of FF into MF.This N,O co-doping strategy for the synthesis of highly efficient catalytic materials with controllable electronic state will provide an excellent opportunity to better understand the structure-function relationship.
基金the financial support from the National Natural Science Foundation of China(U1810111,51872124 and21676116)Natural Science Foundation of Guangdong Province,China(2018B030311010)+1 种基金the Fundamental Research Funds for the Central Universities(21617431)Key Laboratory of Biomass Chemical Engineering of Ministry of Education,Zhejiang University(2018BCE002)
文摘As a renewable biomass-based compound with wide applications in food additives,fine chemical synthesis and fuels,γ-valerolactone(GVL)has attached much attention.While,pyrrolidones are widely used in pharmaceutical,agrochemical,material industrial and other chemical production.In this research,we demonstrated transformations of biomass-based ethyl levulinate(EL)into GVL and pyrrolidones by using heterogeneous catalysts(CNT-Ru-1)with N-heterocyclic carbene ruthenium(NHC-Ru)complex grafted on multi-walled carbon nanotube(CNT).The Ru catalyst showed high efficiency on EL hydrogenation to GVL with both EL conversion and GVL yield exceeding 99%.Moreover,the Ru catalyst readily promoted reductive amination of EL in the presence of various amines for pyrrolidone synthesis.Finally,the Ru catalyst was also applicable to hydrogenation of various carbonyl compounds for the synthesis of the corresponding alcohols with excellent catalytic performance.The research provides insight for heterogenizing the homogeneous noble metal-based catalysts with high catalytic active for biomass-based transformations.
基金We are grateful for the financial support from National Natural Science Foundation of China(U1810111,21676089)Natural Science Foundation of Guangdong Province,China(2018B030311010)+1 种基金Youth Science and Technology Innovation Talent of Guangdong TeZhi Plan(2019TQ05L111)Key Laboratory of Biomass Chemical Engineering of Ministry of Education,Zhejiang University(2018BCE002).
文摘The plasmonic photocatalyst of Pd supported on graphitic carbon nitride(Pd/g-C3N4)exhibits excellent catalytic activity in photo-induced hydrogenation of biomass-based aldehydes with environmental benign reagents of formic acid(HCOOH)as proton source and triethylamine(TEA)as sacrificial electron donator.The chemical and configurational properties of the Pd/g-C3N4 were systematically analyzed with XRD,TEM and XPS.Under optimized conditions,27%yield of furfuryl alcohol with the corresponding turnover frequency(TOF)around 3.72 h^(-1) were obtained from furfural and TEA-HCOOH under visible-light irradiation by using Pd/g-C3N4.Our research additionally reveals that Pd atom is the true catalytic active site for the hydrogenation and the photo-promoted reduction mainly occurs through noble metal nanoparticles(NPs)-induced effect of surface plasmon resonance(SPR).The photo-catalytic system of Pd/g-C3N4 thus demonstrates a green and effective method for the hydrogenation of biomass-based aldehydes with sustainable solar energy as a driven force.
基金Supported by the National Natural Science Foundation of China (21036005) and Scientific and Technology Plan of Zhejiang Province (2011C33016).
文摘Pestalotiopsis sp. J63, producing a high activity of laccase, is a new marine-derived fungus isolated from the oceanic sediment of the East China Sea. Since the marine environment is oligotrophic nutrient, marine derived fungi may use small amount of nutrients to grow and produce laccases. Agricultural residues that are mainly composed of lignin, cellulose and hemicellulose are difficult to be degraded and few microbes can take them as substrates, so they are considered as oligotrophic nutrient and have the potential to be used to produce value added products. In this study, the ability of Pestalotiopsis sp. J63 to use agricultural residues to produce laccases was tested in the submerged fermentation. The combination of 3 g·L 1maltose and 20 g·L 1rice straw was the best carbon sources and 8 g·L 1ammonium sulfate was the best nitrogen source under the condition without inducers. The effects of five inducers, the feeding time and concentration of inducer on laccase production were investigated.Adding 0.09 mmol·L 1phenol after 24 h of incubation led to high laccase activity(5089 U·L 1), while with 0.09mmol·L 1phenol in the medium and wheat bran as the nitrogen source, the laccase activity could reach 5791.7U·L 1. Native-PAGE results showed that two laccase isozymes were present in the cultures. One existed in both induced and non-induced culture filtrates, while the other was only found in the fermentation with the addition of phenol, guaiacol and veratryl alcohol.
基金Supported by the National'Natural Science Foundation of China (20936005, 21076175 and 21076178), the National High Technology Research and Development Program of China (2012AA040211), and the Program for Zhejiang Leading Team of S&T Innovation (2011R50002).
文摘Bioactive natural products are a main source of new drugs,functional foods and food additives.The separation of bioactive natural products plays an important role in transformation and use of biomass.The isolation and purification of bioactive principle from a complex matrix is often inherent bottleneck for the utilization of natural products,so a series of extraction and separation techniques have been developed.This review covers recent advances in the separation of bioactive natural products with an emphasis on their solubility and diffusion coefficients,recent extraction techniques and isolation techniques.This overview of recent technological advances,discussion of pertinent problems and prospect of current methodologies in the separation of bioactive natural products may provide a driving force for development of novel separation techniques.
基金supported by the National High Technology Research and Development Program of China(2009AA044701)the Program for Zhejiang Leading Team of S&T Innovation(2013TD07)
文摘To get deep understanding of the reaction mechanism of coal pyrolysis in hydrogen plasma, the decomposition reaction pathways of aliphatic hydrocarbons and cycloalkanes, which are two main components in volatiles from coal, were investigated. Methane and cyclohexane were chosen as the model compounds. Density functional theory was employed, and many reaction pathways were involved. Calculations were carried out in Gaussian 09 at the B3LYP/6-31G(d,p) level of the theory. The results indicate that the main pyrolysis products of methane and cyclohexane in hydrogen plasma are both hydrogen and acetylene, and the participation of active hydrogen atoms makes dehydrogenation reactions more favorable. H2 mainly comes from dehydrogenation process, while many reaction pathways are responsible for acetylene formation. During coal pyrolysis in hydrogen plasma, three main components in volatiles like aliphatic hydrocarbons, cycloalkanes and aromatic hydrocarbons lead to the formation of hydrogen and acetylene, but their contributions to products distribution are different.
基金Supported by the National Natural Science Foundation of China(No.21376214)
文摘In order to improve the efficient decolorization of dye-containing water by biosorbent and understand the biosorption mechanism, the self-immobilization mycelial pellets were prepared using a marine-derived fungus Aspergillus niger ZJUBE-1, and an azo dye, Congo red was chosen as a model dye to investigate batch decolorization efficiency by pellets. The pellets as biosorbent showed strong salt and acid tolerance in biosorption process. The results for dye adsorption showed that the biosorption process fitted well with models of pseudo-second-order kinetic and Langmuir isotherm, with a maximum adsorption capacity of 263.2 mg·g^(-1) mycelium. During 6 batches of continuous decolorization operation, the mycelial pellets could possess efficient decolorization abilities(>98.5%).The appearance of new peak in the UV–Vis spectral result indicated that the decolorization process may also contain biodegradation. The mechanism studies showed that efficient biosorption ability of pellets only relies on the active zone on the surface of the pellet, which can be enhanced by nutrition supplement or be shifted outward by a reculture process.
基金supported by the National Natural Science Foundation of China(U1162127,U1462201,21076189,21476202 and 21276231)
文摘Hydrogenation of carbazole and N-ethylcarbazole over Raney-Ni catalyst were realized in the temperature range of 393-503 K. 4[H] adduct dominated the hydrogenation products and the formation of 2[H] adduct was the rate-limiting step during the period, in which the conversion of carbazole was less than 40%. The hydrogenation process followed pseudo-first-order kinetics and the hydrogenation activation energies of carbazole and N-ethylcarbazole were 90 k J/mol and 115 k J/mol, respectively. The reaction starting position as well as the pathway of the hydrogenation of(N-ethyl)carbazole were investigated by comparing the kinetic characteristics of hydrogen uptake of carbazole and Nethylcarbazole. The results showed that the reaction was a stepwise hydrogenation process and the first H2 was added to the C1 = C10 double bond in the hydrogenation.
基金supported by Zhejiang Provincial Natural Science Foundation of China(Grant No.LZ12E08002)
文摘Industrial grade multi-walled carbon nanotubes(IG-MWCNTs) are a low-cost substitute for commercially purified multi-walled carbon nanotubes(P-MWCNTs). In this work, IG-MWCNTs were functionalized with tetraethylenepentamine(TEPA) for CO2capture. The TEPA impregnated IG-MWCNTs were characterized with various experimental methods including N2adsorption/desorption isotherms, elemental analysis, X-ray diffraction, Fourier transform infrared spectroscopy and thermogravimetric analysis. Both the adsorption isotherms of IGMWCNTs-n and the isosteric heats of different adsorption capacities were obtained from experiments. TEPA impregnated IG-MWCNTs were also shown to have high CO2adsorption capacity comparable to that of TEPA impregnated P-MWCNTs. The adsorption capacity of IG-MWCNTs based adsorbents was in the range of 2.145 to 3.088 mmol/g, depending on adsorption temperatures. Having the advantages of low-cost and high adsorption capacity, TEPA impregnated IG-MWCNTs seem to be a promising adsorbent for CO2capture from flue gas.
基金financial support from National Natural Science Foundation of China (U1810111)Natural Science Foundation of Guangdong Province, China (2018B030311010)+1 种基金Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Zhejiang University (2018BCE002)the Fundamental Research Funds for the Central Universities (21617431)
文摘This review intends to introduce the application of lignin-derived catalyst for green organic synthesis over latest two decades and aims to present a renewable alternative for conventional catalyst for future industry application. The structure of lignin is initially introduced in this review. Then, various pretreatment and activation technologies of lignin are systematically presented, which includes physical activation for the formation of well-developed porosity and chemical activation to introduce catalytic active sites. Finally, the catalytic performances of various lignin-derived catalysts are rationally assessed and compared with conventional catalysts, which involves lignin-derived solid acids for hydrolysis, hydration, dehydration(trans)esterification, multi-component reaction and condensation, lignin-derived solid base for Knoevenagel reaction, lignin-derived electro-catalysts for electro-oxidation, oxygen reduction reaction, and lignin-derived supported transition metal catalysts for hydrogenation, oxidation, coupling reaction, tandem reaction, condensation reaction, ring-opening reaction, Friedel-Crafts-type reaction,Fischer–Tropsch synthesis, click reaction, Glaser reaction, cycloaddition and(trans)esterification. The above lignin-derived catalysts thus successfully promote the transformations of organic compounds, carbon dioxide, biomass-based cellulose, saccharide and vegetable oil into valuable chemicals and fuels. At the end of this review, some perspectives are given on the current issues and tendency on the lignin-derived catalysts for green chemistry.
文摘The sorption-enhanced steam reforming process of methanol(SESRP-Me OH) to produce high-purity H2 was thermodynamically and experimentally studied.Thermodynamic calculations showed that at a CO2 adsorption ratio of 95%,product gas contains 98.36% H2,32.8 ppm CO under temperature of 130°C and steam-to-methanol(S/M) molar ratio of 2.However,without adsorption-enhanced,the product gas contains nearly 74.99% H2 with 24.96% CO2 and 525 ppm CO.To verify the thermodynamic calculation results,experiments were performed in a fixed-bed reactor loaded with commercial Cu O/Zn O/Al2O3 methanol reforming catalyst and 22% K2CO3-promoted hydrotalcite as CO2 adsorbent.Experimental results showed that 99.61% H2 could be obtained by SESRP-Me OH at reaction temperature of 230°C and S/M of 2.Under the same CH3 OH conversion,the reaction temperature decreased by almost 50°C and H2 concentration increased of more than 20%using SESRP-Me OH compared with solely steam reforming of methanol.The characterization of the adsorbent and catalyst showed that the adsorbent showed good stability while the catalyst was seriously sintered under the high regeneration temperature of the adsorbent.
基金Supported by the National Natural Science Foundation of China(21476198,21576233)the International Science&Technology Cooperation Program of China(2015DFG42070)
文摘Five tryptophan analogues with a hydrophobic indole ring and an amino group on each molecule were used as functional ligands of mixed-mode resins for human serum albumin(HSA) purification. Their adsorption performance was evaluated and the effects of p H and salt addition on HSA adsorption were studied. The resins prepared showed typical p H-dependent adsorption and the highest adsorption capacity and affinity were found at pH 5.0for all the resins tested. The saturated adsorption capacity was 138.02 mg·g^(-1)with the tryptaminefunctionalized resin, which significantly decreased at p H below 4.0 due to electrostatic repulsion between ligands and HSA. Moreover, the addition of Na Cl or(NH_4)_2SO_4in media reduced HSA adsorption capacity, although the two salts showed different affecting profiles. The tryptamine-functionalized resin showed the best salt-tolerant performance, and its high adsorption capacity was maintained under high salt concentrations. In addition, the five resins prepared showed good adsorption selectivity for recombinant HSA from Pichia pastoris broth. Molecular docking results between tryptamine and HSA indicated that tryptamine was favorable to bind on Site II(indole-binding site) of HSA.
基金Project supported by the Special Fund for Basic Scientific Research of Central Colleges,China(Grant No.2012FZA4023)
文摘Current–voltage(I–V) characteristics of hydrogen DC plasma torches with different sizes in an external axial magnetic field under atmospheric pressure are reported.Three anodes with different diameters are adopted in a 50-k W torch:25 mm,30 mm,and 35 mm,respectively.Two different diameters of anodes,that is,100 mm and 130 mm,are adopted in a 1-MW plasma torch.The arc voltage shows a negative trend with the increase of arc current under the operating regimes.On the contrary,arc voltage shows a positive trend as the flow rate of carrier gas increases,and a similar trend is found with increasing the external magnetic flux density.A similarity formula is constructed to correlate the experimental data of the torches mentioned above.Linear fitting shows that the Pearson correlation coefficient is 0.9958.
基金Supported by the National Natural Science Foundation of China(21776243,21476198)the International Science&Technology Cooperation Program of China(2015DFG42070)
文摘The importance of immunoglobulin Y(IgY) as a specific antibody equivalent to mammalian immunoglobulin G(IgG) is well recognized. However, production of highly purified IgY is still difficult due to the lack of specific purification methods. In this study, adsorption behaviors of Ig Y on four mixed-mode resins with functional ligands of 4-mercatoethyl-pyridine(MEP), 2-mercapto-1-methyli-midazole(MMI), 5-aminobenzi-midazole(ABI) and tryptophan-5-aminobenzi-midazole(W-ABI) were evaluated. The results showed that high adsorption ratio were found at p H 6.0–7.0 with little adsorption under acidic conditions. The resin with ABI ligand was then used to separate IgY from immunized chicken serum. An efficient process with Ig Y purity of 95% and recovery of 90% was developed after optimization of loading and elution p H and injection volume. The biological activity of the purified Ig Y was fully maintained. These results indicated that mixed-mode chromatography with specially-designed ligands has great potential for the separation of Ig Y from crude feedstock.
基金supported by Zhejiang Province Welfare Technology Applied Research Project of China(No.2014C31137)National Natural Science Foundation of China(Nos.21436007 and U1462201)the Fundamental Research Funds for the Central Universities of China(No.2015QNA4032)
文摘Pulsed plasma discharge was employed to inactivate bacteria in the injection water for an oil field.The effects of water conductivity and initial concentration of bacteria on elimination efficiency were investigated in the batch and continuous flow modes.It was demonstrated that Fe^(2+) contained in injection water could enhance the elimination efficiency greatly.The addition of reducing agent glutathione(GSH) indicated that active radicals generated by pulsed plasma discharges played an important role in the inactivation of bacteria.Moreover,it was found that the microbial inactivation process for both batch and continuous flow mode well fitted the model based on the Weibull's survival function.