Research On Multi-level Utilization Of Cinnamomum Longepaniculatum Leaves Resources Based On Green Chemistry Concept

Cinnamomum longepaniculatum is the main commercial crops in Yibin,Sichuan,China,and the utilization of C.longepaniculatum leaves was mainly concentrated on extraction essential oil from the leaves of C.longepaniculatum by hydrodistillation before,however,the extraction method performed energy waste,time waste,and efficiency low features,which imposed restrictions on its further applications.The main bioactive compound application of C.longepaniculatum leaves was aimed at the main constituent 1,8-cineole of essential oil,and researches on other bioactive compounds were few reported,especially on multi-level utilization of C.longepaniculatum leaves resources based on green chemistry concept.In this work,innovate bioactive compounds extraction methods were proposed,including to the essential oil,oligomeric and polymeric proanthocyanidins extraction from the leaves of C.longepaniculatum,and the essential oil,oligomeric and polymeric proanthocyanidins application fields were put forward,as well as the leaves of C.longepaniculatum residues after extraction of essential oil,and researches on multi-level utilization of C.longepaniculatum leaves resources were established based on green chemistry concept.The high solid loading enzyme-enhanced pretreatment microwave hydro-distillation(HSEMHD)method was established for extraction essential oil from leaves of C.longepaniculatum.Firstly,based on the monosaccharide compositions of the hydrolysate of C.longepaniculatum leaves analyzed by pre-column derivatization,the optimal cocktail addition was concluded(0.25%pectinase+0.65%cellulase+0.05%hemicellulase+1.05%xylanase)according to the monosaccharide compositions analysis results of C.longepaniculatum leaves cell wall acid hydrolysate and enzyme activites;The optimization condition was analyzed by response surface method,the optimal extraction operation condition was high solid loading of 14%,saponin addition amount of 6 g/L,pH of 5,fermentation temperature of 323.15 K,fermentation time of 6 h,liquid-solid ratio of 24.45 mL/g,microwave irradiation time of 27.41 min,microwave irradiation power of 540 W,and finally obtained essential oil yield of 73.21�2.32 mg/g under the optimal condition;The essential oil constituents in type and content were analyzed by GC-MS,and the main constituent 1,8-cineole of essential oil extracted by HSEMHD was larger than HD,and the essential oil extracted by HSEMHD showed good commercial value.High solid enzymatic pretreatment of C.longepaniculatum leaves has less water consumption,which is in line with the current concept of green sustainable development.Two particle size specifications of controlled-release particles were successfully made by using the gum of Eucommia ulmoides as the natural polymer wall material and essential oil of C.longepaniculatum as the core material by extrusion method.The two types of controlled-release particles features made by 3 mm(3-SRP)and 7 mm(7-SRP)extruder aperture were analyzed,including to physical appearance parameter,appearance,apparent density,drug loading,encapsulation rate,and thermal stability;The sustained-release effects were analyzed under variation temperatures(277.15 K,293.15 K and 333.15 K),and results found that the controlled-release particles 3-SRP and 7-SRP cumulative release variation with time-varying were well fitted by Avrami's equation;The control-release process of the controlled-release particles was the combination of diffusion-limited release and first order kinetic release process under low temperatures(277.15 K and 293.15 K),and first order kinetic release process under high temperature(333.15 K);The two controlled-release particles 3-SRP and 7-SRP were applied in the tomato storage,and the tomato quality features variations were analyzed including to fruit hardness and pulp hardness,insoluble and soluble pectin content,pectin methyllipase(PME)activity and polygalacturonase activity(PG)during storage,and it was found that the addition of controlled-release particles could delay the decreasing tendency of the tomato quality.Researches showed that the controlled-release particles improved the essential oil stability and prolong storage,and showed long time control-release,and they could effectively prolong fruits storage period;Taking the gum of Eucommia ulmoides as one kind new environmentally-friendly degradable wall material in preparation essential oil sustained-release particles was a good choice,and the sustained-release particles showed good controlled release and long-term controlled release properties,Therefore,the natural polymer Eucommia ulmoides gum can be widely appiied in sustained-release particles preparation field.The green solvent of glycine ethyl nitrate([GlyC2]NO3)ionic liquid was successfully synthesis by hydrogen chloride catalysis and displacement reaction methods,and it was applied as extraction solvent for simultaneously extraction oligomeric and polymeric poranthocyanidins(OPC and PPC)from C.longepaniculatum leaves by microwave assisted extraction.Characterization features of the synthesis[GlyC2]NO3 ionic liquid were analyzed by FTIR,DSC and 1H-NMR;The method for preparing[GlyC2]NO3 ionic liquid is simple,workable,and the yield and purity of the product is high,which provides a theoretical basis for the application of amino acid ester ionic liquids as extraction solvent in plant active ingredients extraction field;The total yield of oligomeric and polymeric proanthocyanidins was obtained 11.37�0.44 mg/g under the condition of 2%[GlyC2]NO3 ionic liquid as the extraction solvent,liquid-solid ratio of 20 mL/g,microwave irradiation power of 540 W,and microwave irradiation time of 30 min;After purification and grading of the extract,the recovery of PPC and OPC were 59.98%and 40.02%,respectively,and the average polymerization degrees of OPC and PPC were 2.49 and 12.48,respectively;The extraction kinetic analysis showed that the proanthocyanidins extraction by 70%ethanol and 2%[GlyC2]NO3 ionic liquid from C.longepaniculatum leaves processes were similar in mass transfer process,therefore the[GlyC2]NO3 was showed potential as an alternative or co-solvent of ethanol during extraction plant active ingredients process.Palladium nanoparticles(PdNP)was successfully prepared using the OPC of C.longepaniculatum leaves as plant-derived organic reductant in continuous-flow microtubule under ultrasonic field.The influencing biosynthesis factors were analyzed,and the Pd2+conversion ratio is 89.39%when the OPC and Pd2+volume ratio of 60:40,flow rate of 1 mL/min,ultrasound frequency of 45 kHz,ultrasound power of 200 W,temperature of 333.15 K;The biosynthesis of palladium nanoparticles was characterized and concluded that the biosynthesis of palladium nanoparticles showed the element palladium,good crystallinity,size distribution of 202.86�24.99 nm,purity of 80.94%,irregular polyhedron;The catalytic efficiency of the biosynthesis palladium nanoparticles was tested by methyl orange(MO)and methylene blue(MB)during the process of the photocatalytic degradation,and it performed outstanding;PdNP was successfully prepared using the OPC of C.longepaniculatum leaves as plant-derived organic reductant in continuous-flow microtubule under ultrasonic field,and the preparation process was continuous-flow and controllable,and the reduction condition was mild,and no additional reducing agent was needed,and the PdNP showed good stability.One-way conversion ratio of Pd2+was considered,and high purity of PdNP showed good performance in photocatalytic degradation dye field.We found no same report at home and abroad about this study.The polymeric poranthocyanidins(PPC)of C.longepaniculatum leaves adsorption characteristics in removal of dye from water were discussed.The adsorption influencing factors,adsorption isotherm,adsorption kinetic and adsorption thermodynamic were analyzed in detail,and experimental results showed that the PPC removal of MG process is monolayer chemisorption,and spontaneous endothermic chaos increasing process;FTIR analysis showed that the PPC removal of MG process is owing to electrostatic force(1586 cm-1)and hydrogen bond(3390 cm-1);PPC of C.longepaniculatum leaves is a good adsorbent for removal of environmental pollutants,which could effectively expand efficient and multi-stage utilization of C.longepaniculatum resources.Fe3O4@CLR was prepared by prosoaking and chemical co-precipitation by using the extraction residues of C.longepaniculatum leaves,and the Fe3O4@CLR removal of MG processes were discussed under the static and dynamic(gas-liquid-solid magnetic stabilized bed)conditions.The synthesis Fe3O4@CLR was characterized,and analysis results showed that Fe3O4 particles showed good thermal stability,strong magnetic field response ability,porous;Results showed that the Fe3O4@CLR removal of MG process is monolayer and chemical adsorption,and spontaneous endothermic chaos increasing process;The Fe3O4@CLR removal of MG process was discussed in gas-liquid-solid magnetically stabilized fluidized bed(three-phase system of N2-MG aqueous solution-Fe3O4@CLR particles),and Fe3O4@CLR obtained the equilibrium adsorption capacity of 201.07�10.05 mg/g under the condition of MG initial concentration of 500 mg/L,MG rate flow of 8 mL/min,Fe3O4@CLR mass of 20 g,magnetic intensity of 42.87 Oe.In addition,the Fe3O4@CLR still showed favorable scavenging activity in removal of MG after recycling multiple times;The magnetic porous structure absorbent has a simple preparation method which is easy to operate,and the magnetic porous structure absorbent preparation method can be widely used in the preparation of other types of biomass enzymatic residues in pollution removal fileds;The magnetic adsorbent can be easily separated with the application of MSFB in the magnetic field after adsorption,and the magnetic absorbent can be recycled and reused.This research is the first to strengthen utilization application of the C.longepaniculatum leaves resources based on green chemistry concept.With the goal of green chemical process of terminal less emissions and less pollution,the effective separation of the active ingredients from the C.longepaniculatum leaves and the green chemistry application are realized,which provided the theoretical research basis and technical support for green efficient multi-stage utilization of C.longepaniculatum leaves.