Single-atom catalysts(SACs)are promising for oxygen reduction reaction(ORR)on account of their excellent catalytic activity and maximum utilization of atoms.However,due to the complicated preparation processes and exp...Single-atom catalysts(SACs)are promising for oxygen reduction reaction(ORR)on account of their excellent catalytic activity and maximum utilization of atoms.However,due to the complicated preparation processes and expensive reagents used,the cost of SACs is usually too high to put into practical application.The development of cost-effective and sustainable SACs remains a great challenge.Herein,a low-cost method employing biomass is designed to prepare efficient single-atom Fe-N-C catalysts(SA-Fe-N-C).Benefiting from the confinement effect of porous carbon support and the coordination effect of glucose,SA-Fe-N-C is derived from cheap flour by the two-step pyrolysis.Atomically dispersed Fe atoms exist in the form of Fe-N_(x),which acts as active sites for ORR.The catalyst shows outstanding activity with a half-wave potential(E_(1/2))of 0.86 V,which is better than that of Pt/C(0.84 V).Additionally,the catalyst also exhibits superior stability.The ORR catalyzed by SA-Fe-N-C proceeds via an efficient 4e transfer pathway.The high performance of SA-Fe-N-C also benefits from its porous structure,extremely high specific surface area(1450.1 m^(2)/g),and abundant micropores,which are conducive to increasing the density of active sites and fully exposing them.This work provides a cost-effective strategy to synthesize SACs from cheap biomass,achieving a balance between performance and cost.展开更多
Protoplasts from Candida tropicalis and Candida lipolytica were fused under an optimized electrofusion （electrical pulse strength 6 kV/cm, pulse duration time 40μs and pulse times 5） and then regenerated on YEPD me...Protoplasts from Candida tropicalis and Candida lipolytica were fused under an optimized electrofusion （electrical pulse strength 6 kV/cm, pulse duration time 40μs and pulse times 5） and then regenerated on YEPD media for achieving new genotypes with higher chromium loading capacity. A target fusant RHJ-004 was screened out by its chromium resistance and chromium-sorbing capacity tests for further research. The comparative study of applicability shows that the fusant has better performance than its parent strains in respect of solution pH, biomass concentration and chromium loading capacity. Especially for treating low concentration Cr（VI） （〈20 mg/L）, above 80% chromium is sequestered from the aqueous phase at pH 1-9. Atomic force microscopy （AFM） visualizes the distribution of chromium on the binding sites of the cells, suggesting that the altered surface structure and intracellular constitutes of the fusant associate with its increased biosorption capacity. The rapid biosorption processes of chromium foUow the Langmuir model well.展开更多
Oxygen reduction reaction(ORR)plays a crucial role in many energy storage and conversion devices.Currently,the development of inexpensive and high-performance carbon-based non-precious-metal ORR catalysts in alkaline ...Oxygen reduction reaction(ORR)plays a crucial role in many energy storage and conversion devices.Currently,the development of inexpensive and high-performance carbon-based non-precious-metal ORR catalysts in alkaline media still gains a wide attention.In this paper,the mesoporous Fe-N/C catalysts were synthesized through SiO2-mediated templating method using biomass soybeans as the nitrogen and carbon sources.The SiO2 templates create a simultaneous optimization of both the surface functionalities and porous structures of Fe-N/C catalysts.Detailed investigations indicate that the Fe-N/C3 catalyst prepared with the mass ratio of SiO2 to soybean being 3:4 exhibits brilliant electrocatalytic performance,excellent long-term stability and methanol tolerance for the ORR,with the onset potential and the half-wave potential of the ORR being about 0.890 V and 0.783 V(vs RHE),respectively.Meanwhile,the desired 4-electron transfer pathway of the ORR on the catalysts can be observed.It is significantly proposed that the high BET specific surface area and the appropriate pore-size,as well as the high pyridinic-N and total nitrogen loadings may play key roles in enhancing the ORR performance for the Fe-N/C3 catalyst.These results suggest a feasible route based on the economical and sustainable soybean biomass to develop inexpensive and highly efficient non-precious metal electrochemical catalysts for the ORR.展开更多
Waste cellulosic biomass obtains various applications due to low-cost and eco-benign characteristics.A general strategy is proposed for waste cellulosic biomass to be modified with dialdehyde functional groups as inte...Waste cellulosic biomass obtains various applications due to low-cost and eco-benign characteristics.A general strategy is proposed for waste cellulosic biomass to be modified with dialdehyde functional groups as intermediates through periodate partial oxidation.Finally,aminothiourea-modified waste cellulosic biomass can be prepared through Schiff reaction.Waste corn stalk,cotton and paper as typical precursors,were used to prepare cellulosic biomass,abbreviated as AT-S,AT-C and AT-P,respectively,and their adsorption behaviors of Au(III)from the hydrochloric acid medium were investigated.The pseudo-second kinetics equation as well as the Langmuir isotherm equation can be used to depict the adsorption process,and the maximum adsorption capacities of Au(III)are21.4,19.0and3.28mol/kg for AT-S,AT-C and AT-P at298K,respectively.The adsorption capacities of Au(III)on aminothiourea modified corn stalk(AT-S)is almost357times greater than that of raw corn stalk.To the best of our knowledge,AT-S has the highest adsorption capacity towards Au(III).AT-S also displays a superior separation selectivity towards Au(III)in the presence of Cu(II),Ni(II),Co(II),Pt(VI),Pd(II)and Rh(III).Furthermore,the characterization analysis of XRD,TG,SEM,TEM and FTIR confirms that AuCl4– has been reduced to elemental Au nanoparticles and deposit onto the surface of the biomass.It shows a prospect for waste corn stalk to be used to adsorb Au(III)from liquid phase and the possible fabrication of gold nanoparticles by a general adsorption process without any reductant.展开更多
基金Project(52174338)supported by the National Natural Science Foundation of ChinaProjects(2022JJ20086,2021JJ30796)supported by the Natural Science Foundation of Hunan Province,China+1 种基金Project(2023CXQD005)supported by the Central South University Innovation-Driven Research Programme,ChinaProject(23B0841)supported by the Education Department of Hunan Provincial Government,China。
文摘Single-atom catalysts(SACs)are promising for oxygen reduction reaction(ORR)on account of their excellent catalytic activity and maximum utilization of atoms.However,due to the complicated preparation processes and expensive reagents used,the cost of SACs is usually too high to put into practical application.The development of cost-effective and sustainable SACs remains a great challenge.Herein,a low-cost method employing biomass is designed to prepare efficient single-atom Fe-N-C catalysts(SA-Fe-N-C).Benefiting from the confinement effect of porous carbon support and the coordination effect of glucose,SA-Fe-N-C is derived from cheap flour by the two-step pyrolysis.Atomically dispersed Fe atoms exist in the form of Fe-N_(x),which acts as active sites for ORR.The catalyst shows outstanding activity with a half-wave potential(E_(1/2))of 0.86 V,which is better than that of Pt/C(0.84 V).Additionally,the catalyst also exhibits superior stability.The ORR catalyzed by SA-Fe-N-C proceeds via an efficient 4e transfer pathway.The high performance of SA-Fe-N-C also benefits from its porous structure,extremely high specific surface area(1450.1 m^(2)/g),and abundant micropores,which are conducive to increasing the density of active sites and fully exposing them.This work provides a cost-effective strategy to synthesize SACs from cheap biomass,achieving a balance between performance and cost.
基金Project(NSFC-GDNSF U0933002) supported by the Joint Funds of the National Natural Science Foundation of China and the Natural Science Foundation of Guangdong Province,ChinaProject(50978122) supported by the National Natural Science Foundation of China
文摘Protoplasts from Candida tropicalis and Candida lipolytica were fused under an optimized electrofusion （electrical pulse strength 6 kV/cm, pulse duration time 40μs and pulse times 5） and then regenerated on YEPD media for achieving new genotypes with higher chromium loading capacity. A target fusant RHJ-004 was screened out by its chromium resistance and chromium-sorbing capacity tests for further research. The comparative study of applicability shows that the fusant has better performance than its parent strains in respect of solution pH, biomass concentration and chromium loading capacity. Especially for treating low concentration Cr（VI） （〈20 mg/L）, above 80% chromium is sequestered from the aqueous phase at pH 1-9. Atomic force microscopy （AFM） visualizes the distribution of chromium on the binding sites of the cells, suggesting that the altered surface structure and intracellular constitutes of the fusant associate with its increased biosorption capacity. The rapid biosorption processes of chromium foUow the Langmuir model well.
基金Project(21406273)supported by the National Natural Science Foundation of China
文摘Oxygen reduction reaction(ORR)plays a crucial role in many energy storage and conversion devices.Currently,the development of inexpensive and high-performance carbon-based non-precious-metal ORR catalysts in alkaline media still gains a wide attention.In this paper,the mesoporous Fe-N/C catalysts were synthesized through SiO2-mediated templating method using biomass soybeans as the nitrogen and carbon sources.The SiO2 templates create a simultaneous optimization of both the surface functionalities and porous structures of Fe-N/C catalysts.Detailed investigations indicate that the Fe-N/C3 catalyst prepared with the mass ratio of SiO2 to soybean being 3:4 exhibits brilliant electrocatalytic performance,excellent long-term stability and methanol tolerance for the ORR,with the onset potential and the half-wave potential of the ORR being about 0.890 V and 0.783 V(vs RHE),respectively.Meanwhile,the desired 4-electron transfer pathway of the ORR on the catalysts can be observed.It is significantly proposed that the high BET specific surface area and the appropriate pore-size,as well as the high pyridinic-N and total nitrogen loadings may play key roles in enhancing the ORR performance for the Fe-N/C3 catalyst.These results suggest a feasible route based on the economical and sustainable soybean biomass to develop inexpensive and highly efficient non-precious metal electrochemical catalysts for the ORR.
基金Projects(51504073,51404081,51672275)supported by the National Natural Science Foundation of ChinaProject(2012CBA01202)supported by the National Key Technology Research and Development Program of the Ministry of Science and Technology,China+1 种基金Project(QianJiaoKeHe KY[2015]433)supported by the Research Program of the Education Department of Guizhou Province,ChinaProject(XJG20141104)supported by the Research Program of Talented Scholars of Guizhou Institute of Technology,China
文摘Waste cellulosic biomass obtains various applications due to low-cost and eco-benign characteristics.A general strategy is proposed for waste cellulosic biomass to be modified with dialdehyde functional groups as intermediates through periodate partial oxidation.Finally,aminothiourea-modified waste cellulosic biomass can be prepared through Schiff reaction.Waste corn stalk,cotton and paper as typical precursors,were used to prepare cellulosic biomass,abbreviated as AT-S,AT-C and AT-P,respectively,and their adsorption behaviors of Au(III)from the hydrochloric acid medium were investigated.The pseudo-second kinetics equation as well as the Langmuir isotherm equation can be used to depict the adsorption process,and the maximum adsorption capacities of Au(III)are21.4,19.0and3.28mol/kg for AT-S,AT-C and AT-P at298K,respectively.The adsorption capacities of Au(III)on aminothiourea modified corn stalk(AT-S)is almost357times greater than that of raw corn stalk.To the best of our knowledge,AT-S has the highest adsorption capacity towards Au(III).AT-S also displays a superior separation selectivity towards Au(III)in the presence of Cu(II),Ni(II),Co(II),Pt(VI),Pd(II)and Rh(III).Furthermore,the characterization analysis of XRD,TG,SEM,TEM and FTIR confirms that AuCl4– has been reduced to elemental Au nanoparticles and deposit onto the surface of the biomass.It shows a prospect for waste corn stalk to be used to adsorb Au(III)from liquid phase and the possible fabrication of gold nanoparticles by a general adsorption process without any reductant.
