Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed ...Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.展开更多
It is of great scientific and economic value to recycle waste poly(ethylene terephthalate)(PET)into high-value PET-based metal organic frameworks(MOFs)and further convert it into porous carbon for green energy storage...It is of great scientific and economic value to recycle waste poly(ethylene terephthalate)(PET)into high-value PET-based metal organic frameworks(MOFs)and further convert it into porous carbon for green energy storage applications.In the present study,a facile and costeffective hydrothermal process was developed to direct recycle waste PET bottles into MIL-53(Al)with a 100% conversation,then the MOFderived porous carbon was assembled into electrodes for high-performance supercapacitors.The results indicated that the as-synthesized carbon exhibited high SSA of 1712 m^(2)g^(-1)and unique accordion-like structure with hierarchical porosity.Benefit to these advantageous characters,the assembled three-electrode supercapacitor displayed high specific capacitances of 391 F g^(-1)at the current density of 0.5 A g^(-1)and good rate capability of 73.6% capacitance retention at 20 A g^(-1)in 6 mol L^(-1)KOH electrolyte.Furthermore,the assembled zinc ion capacitor still revealed outstanding capacitance of 335 F g^(-1)at 0.1 A g^(-1),excellent cycling stability of 92.2% capacitance retention after 10000 cycles and ultra-high energy density of 150.3 Wh kg^(-1)at power density of 90 W kg^(-1)in 3 mol L^(-1)ZnSO_(4)electrolyte.It is believed that the current work provides a facile and effective strategy to recycle PET waste into high-valuable MOF,and further expands the applications of MOF-derived carbons for high-performance energy storage devices,so it is conducive to both pollution alleviation and sustainable economic development.展开更多
Fe/N-based biomass porous carbon composite(Fe/N-p Carbon) was prepared by a facile high-temperature carbonization method from biomass,and the effect of Fe/N-p Carbon on the thermal decomposition of energetic molecular...Fe/N-based biomass porous carbon composite(Fe/N-p Carbon) was prepared by a facile high-temperature carbonization method from biomass,and the effect of Fe/N-p Carbon on the thermal decomposition of energetic molecular perovskite-based material DAP-4 was studied.Biomass porous carbonaceous materials was considered as the micro/nano support layers for in situ deposition of Fe/N precursors.Fe/Np Carbon was prepared simply by the high-temperature carbonization method.It was found that it showed the inherent catalysis properties for thermal decomposition of DAP-4.The heat release of DAP-4/Fe/N-p Carbon by DSC curves tested had increased slightly,compared from DAP-4/Fe/N-p Carbon-0.The decomposition temperature peak of DAP-4 at the presence of Fe/N-p Carbon had reduced by 79°C from384.4°C(pure DAP-4) to 305.4°C(DAP-4/Fe/N-p Carbon-3).The apparent activation energy of DAP-4thermal decomposition also had decreased by 29.1 J/mol.The possible catalytic decomposition mechanism of DAP-4 with Fe/N-p Carbon was proposed.展开更多
Dwindling energy sources and a worsening environment are huge global problems,and biomass wastes are an under-exploited source of material for both energy and material generation.Herein,self-template decoction dregs o...Dwindling energy sources and a worsening environment are huge global problems,and biomass wastes are an under-exploited source of material for both energy and material generation.Herein,self-template decoction dregs of Ganoderma lucidum-derived porous carbon nanotubes(ST-DDLGCs)were synthesized via a facile and scalable strategy in response to these challenges.ST-DDLGCs exhibited a large surface area(1731.51 m^(2)g^(-1))and high pore volume(0.76 cm^(3)g^(-1)),due to the interlacing tubular structures of precursors and extra-hierarchical porous structures on tube walls.In the ST-DDLGC/PMS system,the degradation efficiency of capecitabine(CAP)reached~97.3%within 120 min.Moreover,ST-DDLGCs displayed high catalytic activity over a wide pH range of 3–9,and strong anti-interference to these typical and ubiquitous anions in wastewater and natural water bodies(i.e.,H_(2)PO_(4)^(-),NO_(3)^(-),Cl^(-) and HCO_(3)^(-)),in which a ^(1)O_(2)-dominated oxidation was identified and non-radical mechanisms were deduced.Additionally,ST-DDLGC-based coin-type symmetrical supercapacitors exhibited outstanding electrochemical performance,with specific capacitances of up to 328.1 F g^(-1)at 0.5 A g^(-1),and cycling stability of up to 98.6%after 10,000 cycles at a current density of 2 A g^(-1).The superior properties of ST-DDLGCs could be attributed to the unique porous tubular structure,which facilitated mass transfer and presented numerous active sites.The results highlight ST-DDLGCs as a potential candidate for constructing inexpensive and advanced environmentally functional materials and energy storage devices.展开更多
Electrochemical reduction of CO_(2) to syngas(CO and H_(2))offers an efficient way to mitigate carbon emissions and store intermittent renewable energy in chemicals.Herein,the hierarchical one‐dimensional/three‐dime...Electrochemical reduction of CO_(2) to syngas(CO and H_(2))offers an efficient way to mitigate carbon emissions and store intermittent renewable energy in chemicals.Herein,the hierarchical one‐dimensional/three‐dimensional nitrogen‐doped porous carbon(1D/3D NPC)is prepared by carbonizing the composite of Zn‐MOF‐74 crystals in situ grown on a commercial melamine sponge(MS),for electrochemical CO_(2) reduction reaction(CO_(2)RR).The 1D/3D NPC exhibits a high CO/H_(2) ratio(5.06)and CO yield(31 mmol g^(−1)h^(−1))at−0.55 V,which are 13.7 times and 21.4 times those of 1D porous carbon(derived from Zn‐MOF‐74)and N‐doped carbon(carbonized by MS),respectively.This is attributed to the unique spatial environment of 1D/3D NPC,which increases the adsorption capacity of CO_(2) and promotes electron transfer from the 3D N‐doped carbon framework to 1D carbon,improving the reaction kinetics of CO_(2)RR.Experimental results and charge density difference plots indicate that the active site of CO_(2)RR is the positively charged carbon atom adjacent to graphitic N on 1D carbon and the active site of HER is the pyridinic N on 1D carbon.The presence of pyridinic N and pyrrolic N reduces the number of electron transfer,decreasing the reaction kinetics and the activity of CO_(2)RR.The CO/H_(2) ratio is related to the distribution of N species and the specific surface area,which are determined by the degree of spatial confinement effect.The CO/H_(2) ratios can be regulated by adjusting the carbonization temperature to adjust the degree of spatial confinement effect.Given the low cost of feedstock and easy strategy,1D/3D NPC catalysts have great potential for industrial application.展开更多
Catalytic cracking oil slurry is a by-product of catalytic cracking projects,and the efficient conversion and sustainable utilization of this material are issues of continuous concern in the petroleum refining industr...Catalytic cracking oil slurry is a by-product of catalytic cracking projects,and the efficient conversion and sustainable utilization of this material are issues of continuous concern in the petroleum refining industry.In this study,oxygen-enriched activated carbon is prepared using a one-step KOH activation method with catalytic cracking oil slurry as the raw material.The as-prepared oil slurry-based activated carbon exhibits a high specific surface area of 2102 m^(2)/g,welldefined micropores with an average diameter of 2 nm,and a rich oxygen doping content of 32.97%.The electrochemical performance of the nitrogen-doped porous carbon is tested in a three-electrode system using a 6 mol/L KOH solution as the electrolyte.It achieves a specific capacitance of up to 230 F/g at a current density of 1 A/g.Moreover,the capacitance retention rate exceeds 89%after 10000 charge and discharge cycles,demonstrating excellent cycle stability.This method not only improves the utilization efficiency of industrial fuel waste but also reduces the production cost of supercapacitor electrode materials,thereby providing a simple and effective strategy for the resource utilization of catalytic cracking oil slurries.展开更多
Lignin-derived porous carbons have emerged as promising electrode materials for supercapacitors.However,the challenge remains in designing and controlling their structure to achieve ideal electrochemical performance d...Lignin-derived porous carbons have emerged as promising electrode materials for supercapacitors.However,the challenge remains in designing and controlling their structure to achieve ideal electrochemical performance due to the complex molecular structure of lignin and its intricate chemical reactions during the activation process.In this study,three porous carbons were synthesized from lignin by spray drying and chemical activation with vary-ing KOH ratios.The specific surface area and structural order of the prepared porous carbon continued to increase with the increase of the KOH ratio.Thermogravimetric-mass spectrometry(TG-MS)was employed to track the molecular fragments generated during the pyrolysis of KOH-activated lignin,and the mechanism of the thermochemical conversion was investigated.During the thermochemical conversion of lignin,KOH facili-tated the removal of H2 and CO,leading to the formation of not only more micropores and mesopores,but also more ordered carbon structures.The pore structure exhibited a greater impact than the carbon structure on the electrochemical performance of porous carbon.The optimized porous carbon exhibited a capacitance of 256 F g-1 at a current density of 0.2 A g-1,making it an ideal electrode material for high-performance supercapacitors.展开更多
Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged inter...Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged interlayer spacing,abundant defects,and favorable mesoporous structures.The structural changes of NPCNs in potassiation and depotassiation processes are analyzed by using Raman spectroscopy and transmission electron microscopy.Due to the unique structure of NPCNs,the PIHC device assembled using NPCNs as both the anode and cathode material(double-functional self-matching material)exhibits a superior energy density of 128 Wh kg^(-1)with a capacity retention of 90.8%after 9000 cycles.This research can promote the development of double-functional self-matching materials for hybrid energy storage devices with ultra-high performance.展开更多
Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this...Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.展开更多
Considering their superior theoretical capacity and low voltage plateau,bismuth(Bi)-based materials are being widely explored for application in potassium-ion batteries(PIBs).Unfortunately,pure Bi and Bibased compound...Considering their superior theoretical capacity and low voltage plateau,bismuth(Bi)-based materials are being widely explored for application in potassium-ion batteries(PIBs).Unfortunately,pure Bi and Bibased compounds suffer from severe electrochemical polarization,agglomeration,and dramatic volume fluctuations.To develop an advanced bismuth-based anode material with high reactivity and durability,in this work,the pyrolysis of Bi-based metal-organic frameworks and in-situ selenization techniques have been successfully used to produce a Bi-based composite with high capacity and unique structure,in which Bi/Bi_(3)Se_(4)nanoparticles are encapsulated in carbon nanorods(Bi/Bi_(3)Se_(4)@CNR).Applied as the anode material of PIBs,the Bi/Bi_(3)Se_(4)@CNR displays fast potassium storage capability with 307.5 m A h g^(-1)at 20 A g^(-1)and durable cycle performance of 2000 cycles at 5 A g^(-1).Notably,the Bi/Bi_(3)Se_(4)@CNR also showed long cycle stability over 1600 cycles when working in a full cell system with potassium vanadate as the cathode material,which further demonstrates its promising potential in the field of PIBs.Additionally,the dual potassium storage mechanism of the Bi/Bi_(3)Se_(4)@CNR based on conversion and alloying reaction has also been revealed by in-situ X-ray diffraction.展开更多
The low-cost and efficient elimination of tetracycline from wastewater and to decrease the concentration in soils,sediments,rivers,underground water,or lakes are crucial to human health.Herein,threedimensional porous ...The low-cost and efficient elimination of tetracycline from wastewater and to decrease the concentration in soils,sediments,rivers,underground water,or lakes are crucial to human health.Herein,threedimensional porous carbon nanomaterials were synthesized using glucose and NH_(4)Cl by sugarblowing process at 900℃ and then oxidized under air atmosphere for surface functional group modification.The prepared 3D porous carbon nanomaterials were applied for the removal of tetracycline from aqueous solutions.The sorption isotherms were well simulated by the Langmuir model,with the calculated sorption capacity of 2378 mg·g^(-1) for C-450 at pH=6.5,which was the highest value of today's reported materials.The porous carbon nanomaterials showed high stability at acidic conditions and selectivity in high salt concentrations.The good recycle ability and high removal efficiency of tetracycline from natural groundwater indicated the potential application of the porous carbon nanomaterials in natural environmental antibiotic pollution cleanup.The outstanding sorption properties were attributed to the structures,surface areas and functional groups,strong interactions such as H-bonding,π-π interaction,electrostatic attraction,etc.This paper highlighted the synthesis of porous carbon nanomaterials with high specific surfaces,high sorption capacities,stability,and reusability in organic chemicals'pollution treatment.展开更多
Citral(Eo)exhibits excellent fungicidal activities.However,it is difficult to maintain long-term fungicidal activity due to its strong volatility.Herein,a controlled-release strategy by using biomass-derived porous ca...Citral(Eo)exhibits excellent fungicidal activities.However,it is difficult to maintain long-term fungicidal activity due to its strong volatility.Herein,a controlled-release strategy by using biomass-derived porous carbon(BC)was developed to overcome the drawback of Eo.New composite materials were prepared by loading Eo on tea stem porous carbon(BC@Eo),and their controlled-release fungicidal activity against Exobasidium vexans was assessed.BC with a large specific surface area of 1001.6 m2/g and mesoporous structure was fabricated through carbonization tempera-ture of 700℃.The BC@Eo materials were characterized using Fourier-transform infrared spectroscopy and X-ray powder diffraction.The results suggested that chemical and physical interactions occurred in BC@Eo.The Eo release profile suggested a biphasic pattern with an initial fast release on days 1–14 and a subsequent controlled phase on days 14–30.The in vitro cumulative release percentage of Eo from BC@Eo was 51%during one month,and this result was significantly lower than that from free Eo(cumulative release percentage of Eo of 82%in one week).The anti-fungal activities of Eo and BC@Eo against E.vexans were determined using the inhibition zone method.The results indicated that Eo and BC@Eo formed large inhibition zones of 19.66±0.79 and 21.92±0.77 mm,respectively.The influence on the hyphal structure of E.vexans was observed by scanning electron microscopy on day 30.The hyphal structure of E.vexans treated with BC@Eo was more shrunken than that treated with Eo at 30 days,suggesting that BC@Eo prolongs the fungicidal activity against E.vexans.This study demonstrated that the encapsulation of Eo in BC for developing the BC@Eo materials could be a promising strategy to inhibit volatility and maintain the fungicidal activity of Eo and provide a potential alternative for the reuse of abundant tea biomass waste resources.展开更多
In-situ MgO-doped ordered mesoporous carbon(OMC@MgO)was fabricated by formaldehyde-free self-assembly method,in which biomass-derived tannin was used as carbon precursor replacing fossil-based phenolics,Mg^(2+)as both...In-situ MgO-doped ordered mesoporous carbon(OMC@MgO)was fabricated by formaldehyde-free self-assembly method,in which biomass-derived tannin was used as carbon precursor replacing fossil-based phenolics,Mg^(2+)as both cross-linker and precursor of catalytic sites.Up to~20 wt% MgO could be doped in the carbon skeleton with good dispersion retaining well-ordered mesoporous structures,while more MgO content(35 wt%)led to the failing in the formation of ordered mesoporous structure.The OMC@MgO possessed a high specific surface area(298.8 m^(2) g^(-1)),uniform pore size distribution(4.8 nm)and small crystallite size of MgO(1.73 nm)due to the confinement effect of ordered mesoporous structure.Using OMC@MgO as the heterogeneous catalyst,a maximum fructose yield of 32.4% with a selectivity up to 81.1%was achieved from glucose in water(90℃,60 min),which is much higher than that obtained using the MgO doped active carbon via conventional post-impregnation method(26.5%yield with 58.3% selectivity).Higher reaction temperature(>90℃)resulted in decrease of selectivity due to the formation of humins.The designed OMC@MgO displayed tolerant to high initial glucose concentrations(10 wt%)and could remain good recyclability without significant loss of activity for three cycles.展开更多
Doping heteroatoms on carbon materials could bring some special advantages for using as catalyst support.In this work, a boron doped lamellar porous carbon(B-LPC) was prepared facilely and utilized as carbonbased supp...Doping heteroatoms on carbon materials could bring some special advantages for using as catalyst support.In this work, a boron doped lamellar porous carbon(B-LPC) was prepared facilely and utilized as carbonbased support to construct Cu/B-LPC catalyst for dimethyl oxalate(DMO) hydrogenation. Doping boron could make the B-LPC own more defects on surface and bigger pore size than B-free LPC, which were beneficial to disperse and anchor Cu nanoparticles. Moreover, the interaction between Cu species and B-LPC could be strengthened by the doped B, which not only stabilized the Cu nanoparticles, but also tuned the valence of Cu species to maintain more Cu^(+). Therefore, the B-doped Cu/B-LPC catalyst exhibited stronger hydrogenation ability and obtained higher alcohols selectivity than Cu/LPC, as well as high stability without decrease of DMO conversion and ethylene glycol selectivity even after 300 h of reaction at 240℃.展开更多
Common strategies for catalytic graphitization of biochar into graphitic porous carbon(GPC)still face great challenges,such as the realization of simple procedures,energy conservation,and green processes.Controlling o...Common strategies for catalytic graphitization of biochar into graphitic porous carbon(GPC)still face great challenges,such as the realization of simple procedures,energy conservation,and green processes.Controlling over the graphitization degree and pore structure of biochar is the key to its structural diversification.Herein,a clean and energy-efficient method is developed to synthesize adjustable graphitic degree and structure porosity GPC from rice husk-based carbon(RHC)at a relatively low temperature of 800–1000°C with environment-benign organometallic catalyst ethylenediaminetetraacetic acid ferric sodium salt(EDTA-iron)and the recovery ratio of catalyst is as high as 97%.The formed by the organic ligands of EDTA-iron facilitates the etching of RHC surface and pore by iron,resulting in highly graphitized and developed porous GPCs.The pore structure and graphitization degree of GPCs can be adjusted by altering the catalyst loading,temperature,and holding time.The catalyst EDTA-iron with a lower concentration mainly plays the role of etching,which promotes the formation of porous carbon with larger surface area(SBET=1187.2 m^(2)·g^(-1)).The catalyst with higher concentration mainly plays the role of catalyzing graphitization and promotes the obtaining of graphitic carbon with high graphitization degree(ID/IG=0.19).The mechanism of EDTA-iron catalyzed graphitization of RHC is explored by the comprehensive analysis of BET,XRD,Raman,TEM and TGA.This research not only provides an efficient method for the preparation of high-quality biomass-based graphite carbon,but also provides a feasible method for the preparation of biomass-based porous carbon.展开更多
Rational design and exploration of low-cost and robust bifunctional oxygen electrocatalysts are vitally important for developing high-performance zinc-air batteries(ZABs).Herein,we reported a facile yet cost-efficient...Rational design and exploration of low-cost and robust bifunctional oxygen electrocatalysts are vitally important for developing high-performance zinc-air batteries(ZABs).Herein,we reported a facile yet cost-efficient approach to construct a bifunctional oxygen reduction reaction(ORR)/oxygen evolution reaction(OER)electrocatalyst composed of N-doped porous carbon nanosheet flowers decorated with Fe Co nanoparticles(Fe Co/N-CF).Rational design of this catalyst is achieved by designing Schiff-base polymer with unique molecular structure via hydrogen bonding of cyanuramide and terephthalaldehyde polycondensate in the presence of metal cations.It exhibits excellent activity and stability for electrocatalysis of ORR/OER,enabling ZAB with a high peak power density of 172 m W cm^(-2)and a large specific capacity of 811 m A h g^(-1)Znat large current.The rechargeable ZAB demonstrates excellent durability for 1000 h with slight voltage decay,far outperforming a couple of precious Pt/Ir-based catalysts.Density functional theory(DFT)calculations reveal that high activity of bimetallic Fe Co stems from enhanced O_(2)and OH-adsorption and accelerated O_(2)dissociation by OAO bond activation.展开更多
In order to deal with the increasingly serious environmental problems,it is important and necessary to lower the concentration of greenhouse gases,especially the CO_(2)gas.CO_(2)capture and storage are the relative su...In order to deal with the increasingly serious environmental problems,it is important and necessary to lower the concentration of greenhouse gases,especially the CO_(2)gas.CO_(2)capture and storage are the relative suitable options for the reduction of these harmful gas concentration.Through the variation of mass ratio of KOH to bio-char,the as prepared active carbon PC-4 exhibits a higher specific surface area of 2491.57 cm^(3)·g^(−1),with the ultra-micropores of 0.5 and 1.2 nm.At 298 K/1 bar,the CO_(2)adsorption capacity of PC-4 also represents the highest value of 5.81 mmol/g.This work demonstrates that the both the pore size and the specific surface area are equally important to enhance the CO_(2)adsorption.This work provides a sustainable method to develop high efficiency waste-based adsorbents to deal with environmental issues of CO_(2)gas.展开更多
Continuous accumulation and emission into the atmosphere of anthropogenic carbon dioxide(CO_(2)),a major greenhouse gas,has been recognized as a primary contributor to climate change associated with the global warming...Continuous accumulation and emission into the atmosphere of anthropogenic carbon dioxide(CO_(2)),a major greenhouse gas,has been recognized as a primary contributor to climate change associated with the global warming and acidification of oceans.This has led to drastic changes in the natural ecosystem,and hence an unhealthy ecological environment for human society.Thus,the effective mitigation of the ever increasing CO_(2)emission has been recognized as the most important global challenge.To achieve zero carbon footprint,novel materials and approaches are required for potentially reducing the CO_(2)release,while our current fossil-fuel-based energy must be replaced by renewable energy free from emissions.In this paper,porous carbons with hierarchical pore structures are promising for CO_(2)adsorption and electrochemical CO_(2)reduction owing to their high specific surface area,excellent catalytic performance,low cost and long-term stability.Since efficient gas-phased(electro)catalysis involves the access of reactants to active sites at the gas-liquid-solid triple phase,the hierarchical porous carbon materials possess multiple advantages for various CO_(2)-related applications with enhanced volumetric and gravimetric activities(e.g.,CO_(2)uptake and current density)for practical operations.Recent studies have demonstrated that porous carbon materials exhibited notable activities as CO_(2)adsorbents and provided facile conducting pathways and mass diffusion channels for efficient electrochemical CO_(2)reduction even under the high current operation conditions.Herein,we summarize recent advances in porous carbon materials for CO_(2)capture,storage,and electrochemical conversion.Prospectives and challenges on the rational design of porous carbon materials for scalable and practical CO_(2)capture and conversion are also discussed.展开更多
With the emergence of supercapacitors(SCs),the creation of bio-based electrode materials has grown in significance for the advancement of energy storage.However,it is particularly difficult for cathode materials to me...With the emergence of supercapacitors(SCs),the creation of bio-based electrode materials has grown in significance for the advancement of energy storage.However,it is particularly difficult for cathode materials to meet the demands of practical uses due to their low energy density.Herein,MIL-88 was fabricated in situ on the surface of cotton fibers used in cosmetics,followed by creating Fe_(2)N@porous carbon fiber composite(Fe_(2)N@PCF)through heat treatment at various temperatures.Fe_(2)N@PCF-800 demonstrates excellent specific capacitance performance(552 F g^(-1) at 1 A g^(-1)).Meanwhile,The AC//Fe_(2)N@PCF-800 device exhibits the largest energy density of 38 Wh kg^(-1) at 800 W kg^(-1) and a long cycling stability(83.3%capacity retention after 6000 cycles).Our elaborately designed Fe_(2)N@PCF demonstrate multiple advantages:i)the Fe_(2)N@PCF-800 shows abundant mesopores,providing abundant ion-diffusion pathways for mass transport and rich graphite microstructures,improving electrical conductivity for electron transferowning;ii)the rich nitrogen dopants and Fe_(2)N structure within all carbon components increase the capacitance through their pseudocapacitive contribution.These findings highlight the importance of biomass derived carbon materials for SCs applications.展开更多
The hierarchically porous carbons (HPCs) were prepared by sol-gel selassembly technology in different surfactant concentrations and were used as the potential electrode for lithium oxygen batteries. The physical and...The hierarchically porous carbons (HPCs) were prepared by sol-gel selassembly technology in different surfactant concentrations and were used as the potential electrode for lithium oxygen batteries. The physical and electrochemical properties of the as-prepared HPCs were investigated by filed emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), nitrogen adsorption-desorption isotherm and galvanostatic charge/discharge. The results indicate that all of the HPCs mainly possess mesoporous structure with nearly similar pore size distribution. Using the HPCs as the electrode, a high discharge capacity for lithium oxygen battery can be achieved, and the discharge capacity increases with the specific surface area. Especially, the HPCs-3 oxygen electrode with CTAB concentration of 0.27 mol/L exhibits good capacity retention through controlling discharge depth to 800 mA·h/g and the highest discharge capacity of 2050 mA·h/g at a rate of 0.1 mA/cm2.展开更多
基金the National Natural Science Foundation of China(Nos.52102036 and52301192)the Sichuan Science and Technology Program,China(No.2021JDRC0099)+3 种基金Taishan Scholars and Young Experts Program of Shandong Province,China(No.tsqn202103057)the Qingchuang Talents Induction Program of Shandong Higher Education Institution,China(Research and Innovation Team of Structural-Functional Polymer Composites)Special Financial of Shandong Province,China(Structural Design of High-efficiency Electromagnetic Wave-absorbing Composite Materials and Construction of Shandong Provincial Talent Teams)“Sanqin Scholars”Innovation Teams Project of Shaanxi Province,China(Clean Energy Materials and High-Performance Devices Innovation Team of Shaanxi Dongling Smelting Co.,Ltd.)。
文摘Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.
基金the financial support from the NCN,Poland,UMO-2020/39/B/ST8/02937 and NAWA,2020 PPN/BEK/2020/1/00129/ZAS/00001support from the Institute for Basic Science(IBS-R019-D1)。
文摘It is of great scientific and economic value to recycle waste poly(ethylene terephthalate)(PET)into high-value PET-based metal organic frameworks(MOFs)and further convert it into porous carbon for green energy storage applications.In the present study,a facile and costeffective hydrothermal process was developed to direct recycle waste PET bottles into MIL-53(Al)with a 100% conversation,then the MOFderived porous carbon was assembled into electrodes for high-performance supercapacitors.The results indicated that the as-synthesized carbon exhibited high SSA of 1712 m^(2)g^(-1)and unique accordion-like structure with hierarchical porosity.Benefit to these advantageous characters,the assembled three-electrode supercapacitor displayed high specific capacitances of 391 F g^(-1)at the current density of 0.5 A g^(-1)and good rate capability of 73.6% capacitance retention at 20 A g^(-1)in 6 mol L^(-1)KOH electrolyte.Furthermore,the assembled zinc ion capacitor still revealed outstanding capacitance of 335 F g^(-1)at 0.1 A g^(-1),excellent cycling stability of 92.2% capacitance retention after 10000 cycles and ultra-high energy density of 150.3 Wh kg^(-1)at power density of 90 W kg^(-1)in 3 mol L^(-1)ZnSO_(4)electrolyte.It is believed that the current work provides a facile and effective strategy to recycle PET waste into high-valuable MOF,and further expands the applications of MOF-derived carbons for high-performance energy storage devices,so it is conducive to both pollution alleviation and sustainable economic development.
基金National Natural Science Foundation of China(Grant No.21975227)the Found of National defence Science and Technology Key Laboratory (Grant No.6142602210306)。
文摘Fe/N-based biomass porous carbon composite(Fe/N-p Carbon) was prepared by a facile high-temperature carbonization method from biomass,and the effect of Fe/N-p Carbon on the thermal decomposition of energetic molecular perovskite-based material DAP-4 was studied.Biomass porous carbonaceous materials was considered as the micro/nano support layers for in situ deposition of Fe/N precursors.Fe/Np Carbon was prepared simply by the high-temperature carbonization method.It was found that it showed the inherent catalysis properties for thermal decomposition of DAP-4.The heat release of DAP-4/Fe/N-p Carbon by DSC curves tested had increased slightly,compared from DAP-4/Fe/N-p Carbon-0.The decomposition temperature peak of DAP-4 at the presence of Fe/N-p Carbon had reduced by 79°C from384.4°C(pure DAP-4) to 305.4°C(DAP-4/Fe/N-p Carbon-3).The apparent activation energy of DAP-4thermal decomposition also had decreased by 29.1 J/mol.The possible catalytic decomposition mechanism of DAP-4 with Fe/N-p Carbon was proposed.
基金financial support from the National Natural Science Foundation of China(21908024,22078374 and 52100173)Key Realm Research and Development Program of Guangdong Province(2020B0202080001)+2 种基金Science and Technology Planning Project of Guangdong Province,China(2021B1212040008)Guangdong Laboratory for Lingnan Modern Agriculture Project(NT2021010)Scientific and Technological Planning Project of Guangzhou(202206010145).
文摘Dwindling energy sources and a worsening environment are huge global problems,and biomass wastes are an under-exploited source of material for both energy and material generation.Herein,self-template decoction dregs of Ganoderma lucidum-derived porous carbon nanotubes(ST-DDLGCs)were synthesized via a facile and scalable strategy in response to these challenges.ST-DDLGCs exhibited a large surface area(1731.51 m^(2)g^(-1))and high pore volume(0.76 cm^(3)g^(-1)),due to the interlacing tubular structures of precursors and extra-hierarchical porous structures on tube walls.In the ST-DDLGC/PMS system,the degradation efficiency of capecitabine(CAP)reached~97.3%within 120 min.Moreover,ST-DDLGCs displayed high catalytic activity over a wide pH range of 3–9,and strong anti-interference to these typical and ubiquitous anions in wastewater and natural water bodies(i.e.,H_(2)PO_(4)^(-),NO_(3)^(-),Cl^(-) and HCO_(3)^(-)),in which a ^(1)O_(2)-dominated oxidation was identified and non-radical mechanisms were deduced.Additionally,ST-DDLGC-based coin-type symmetrical supercapacitors exhibited outstanding electrochemical performance,with specific capacitances of up to 328.1 F g^(-1)at 0.5 A g^(-1),and cycling stability of up to 98.6%after 10,000 cycles at a current density of 2 A g^(-1).The superior properties of ST-DDLGCs could be attributed to the unique porous tubular structure,which facilitated mass transfer and presented numerous active sites.The results highlight ST-DDLGCs as a potential candidate for constructing inexpensive and advanced environmentally functional materials and energy storage devices.
基金National Natural Science Foundation of China,Grant/Award Numbers:51873085,52071171,52202248The Australian Government through the Cooperative Research Centres Projects,Grant/Award Number:CRCPⅩⅢ000077+10 种基金Linkage Project,Grant/Award Numbers:LP210100467,LP210200345,LP210200504,LP220100088Natural Science Foundation of Liaoning Province‐Outstanding Youth Foundation,Grant/Award Number:2022‐YQ‐14Discovery Project,Grant/Award Number:DP220100603China Scholarship Council(CSC Scholarship),Grant/Award Number:202006800009Liaoning Revitalization Talents Program,Grant/Award Number:XLYC2007056Australian Research Council(ARC)through Future Fellowship,Grant/Award Numbers:FT210100298,FT210100806Shenyang Science and Technology Project,Grant/Award Number:21‐108‐9‐04Industrial Transformation Training Centre schemes,Grant/Award Number:IC180100005Natural Science Foundation of Liaoning Province,Grant/Award Number:2020‐MS‐137Key Research Project of Department of Education of Liaoning Province,Grant/Award Number:LJKZZ20220015Liaoning BaiQianWan Talents Program,Grant/Award Number:LNBQW2018B0048。
文摘Electrochemical reduction of CO_(2) to syngas(CO and H_(2))offers an efficient way to mitigate carbon emissions and store intermittent renewable energy in chemicals.Herein,the hierarchical one‐dimensional/three‐dimensional nitrogen‐doped porous carbon(1D/3D NPC)is prepared by carbonizing the composite of Zn‐MOF‐74 crystals in situ grown on a commercial melamine sponge(MS),for electrochemical CO_(2) reduction reaction(CO_(2)RR).The 1D/3D NPC exhibits a high CO/H_(2) ratio(5.06)and CO yield(31 mmol g^(−1)h^(−1))at−0.55 V,which are 13.7 times and 21.4 times those of 1D porous carbon(derived from Zn‐MOF‐74)and N‐doped carbon(carbonized by MS),respectively.This is attributed to the unique spatial environment of 1D/3D NPC,which increases the adsorption capacity of CO_(2) and promotes electron transfer from the 3D N‐doped carbon framework to 1D carbon,improving the reaction kinetics of CO_(2)RR.Experimental results and charge density difference plots indicate that the active site of CO_(2)RR is the positively charged carbon atom adjacent to graphitic N on 1D carbon and the active site of HER is the pyridinic N on 1D carbon.The presence of pyridinic N and pyrrolic N reduces the number of electron transfer,decreasing the reaction kinetics and the activity of CO_(2)RR.The CO/H_(2) ratio is related to the distribution of N species and the specific surface area,which are determined by the degree of spatial confinement effect.The CO/H_(2) ratios can be regulated by adjusting the carbonization temperature to adjust the degree of spatial confinement effect.Given the low cost of feedstock and easy strategy,1D/3D NPC catalysts have great potential for industrial application.
基金the National Natural Science Foundation of China(52206262)Small and Medium-sized Sci-tech Enterprises Innovation Capability Improvement Project of Shandong Province,China(2022TSGC2248,2023TSGC0579)+1 种基金Talent Research Project of Qilu University of Technology(Shandong Academy of Sciences)(2023RCKY170)Natural Science Foundation of Shandong Province,China(ZR2020ME191).
文摘Catalytic cracking oil slurry is a by-product of catalytic cracking projects,and the efficient conversion and sustainable utilization of this material are issues of continuous concern in the petroleum refining industry.In this study,oxygen-enriched activated carbon is prepared using a one-step KOH activation method with catalytic cracking oil slurry as the raw material.The as-prepared oil slurry-based activated carbon exhibits a high specific surface area of 2102 m^(2)/g,welldefined micropores with an average diameter of 2 nm,and a rich oxygen doping content of 32.97%.The electrochemical performance of the nitrogen-doped porous carbon is tested in a three-electrode system using a 6 mol/L KOH solution as the electrolyte.It achieves a specific capacitance of up to 230 F/g at a current density of 1 A/g.Moreover,the capacitance retention rate exceeds 89%after 10000 charge and discharge cycles,demonstrating excellent cycle stability.This method not only improves the utilization efficiency of industrial fuel waste but also reduces the production cost of supercapacitor electrode materials,thereby providing a simple and effective strategy for the resource utilization of catalytic cracking oil slurries.
基金funding from the Key Research and Development Projects of Zhejiang Province(2022C01236)and the Ningbo Top Talent Project.
文摘Lignin-derived porous carbons have emerged as promising electrode materials for supercapacitors.However,the challenge remains in designing and controlling their structure to achieve ideal electrochemical performance due to the complex molecular structure of lignin and its intricate chemical reactions during the activation process.In this study,three porous carbons were synthesized from lignin by spray drying and chemical activation with vary-ing KOH ratios.The specific surface area and structural order of the prepared porous carbon continued to increase with the increase of the KOH ratio.Thermogravimetric-mass spectrometry(TG-MS)was employed to track the molecular fragments generated during the pyrolysis of KOH-activated lignin,and the mechanism of the thermochemical conversion was investigated.During the thermochemical conversion of lignin,KOH facili-tated the removal of H2 and CO,leading to the formation of not only more micropores and mesopores,but also more ordered carbon structures.The pore structure exhibited a greater impact than the carbon structure on the electrochemical performance of porous carbon.The optimized porous carbon exhibited a capacitance of 256 F g-1 at a current density of 0.2 A g-1,making it an ideal electrode material for high-performance supercapacitors.
基金financially supported by the National Natural Science Foundation of China(Nos.21873026,21573061,21773059)。
文摘Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged interlayer spacing,abundant defects,and favorable mesoporous structures.The structural changes of NPCNs in potassiation and depotassiation processes are analyzed by using Raman spectroscopy and transmission electron microscopy.Due to the unique structure of NPCNs,the PIHC device assembled using NPCNs as both the anode and cathode material(double-functional self-matching material)exhibits a superior energy density of 128 Wh kg^(-1)with a capacity retention of 90.8%after 9000 cycles.This research can promote the development of double-functional self-matching materials for hybrid energy storage devices with ultra-high performance.
基金financial support from projects funded by the National Natural Science Foundation of China(22179017,52172038).
文摘Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.
基金financially supported by the National Natural Science Foundation of China (22209057)the Guangdong Basic and Applied Basic Research Foundation (2021A1515010362)+1 种基金the Guangzhou Basic and Applied Basic Research Foundation (202102020995)the Open Fund of Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications (2020B121201005)。
文摘Considering their superior theoretical capacity and low voltage plateau,bismuth(Bi)-based materials are being widely explored for application in potassium-ion batteries(PIBs).Unfortunately,pure Bi and Bibased compounds suffer from severe electrochemical polarization,agglomeration,and dramatic volume fluctuations.To develop an advanced bismuth-based anode material with high reactivity and durability,in this work,the pyrolysis of Bi-based metal-organic frameworks and in-situ selenization techniques have been successfully used to produce a Bi-based composite with high capacity and unique structure,in which Bi/Bi_(3)Se_(4)nanoparticles are encapsulated in carbon nanorods(Bi/Bi_(3)Se_(4)@CNR).Applied as the anode material of PIBs,the Bi/Bi_(3)Se_(4)@CNR displays fast potassium storage capability with 307.5 m A h g^(-1)at 20 A g^(-1)and durable cycle performance of 2000 cycles at 5 A g^(-1).Notably,the Bi/Bi_(3)Se_(4)@CNR also showed long cycle stability over 1600 cycles when working in a full cell system with potassium vanadate as the cathode material,which further demonstrates its promising potential in the field of PIBs.Additionally,the dual potassium storage mechanism of the Bi/Bi_(3)Se_(4)@CNR based on conversion and alloying reaction has also been revealed by in-situ X-ray diffraction.
基金Financial support from the National Natural Science Foundation of China(22276054)。
文摘The low-cost and efficient elimination of tetracycline from wastewater and to decrease the concentration in soils,sediments,rivers,underground water,or lakes are crucial to human health.Herein,threedimensional porous carbon nanomaterials were synthesized using glucose and NH_(4)Cl by sugarblowing process at 900℃ and then oxidized under air atmosphere for surface functional group modification.The prepared 3D porous carbon nanomaterials were applied for the removal of tetracycline from aqueous solutions.The sorption isotherms were well simulated by the Langmuir model,with the calculated sorption capacity of 2378 mg·g^(-1) for C-450 at pH=6.5,which was the highest value of today's reported materials.The porous carbon nanomaterials showed high stability at acidic conditions and selectivity in high salt concentrations.The good recycle ability and high removal efficiency of tetracycline from natural groundwater indicated the potential application of the porous carbon nanomaterials in natural environmental antibiotic pollution cleanup.The outstanding sorption properties were attributed to the structures,surface areas and functional groups,strong interactions such as H-bonding,π-π interaction,electrostatic attraction,etc.This paper highlighted the synthesis of porous carbon nanomaterials with high specific surfaces,high sorption capacities,stability,and reusability in organic chemicals'pollution treatment.
基金Supported by National Modern Agricultural Industry Technology System,Youth Science and Technology Fund of Guizhou Academy of Agricultural Sciences No.[2020]02,Guiding Project of Guizhou Academy of Agricultural Sciences No.[2018]01.
文摘Citral(Eo)exhibits excellent fungicidal activities.However,it is difficult to maintain long-term fungicidal activity due to its strong volatility.Herein,a controlled-release strategy by using biomass-derived porous carbon(BC)was developed to overcome the drawback of Eo.New composite materials were prepared by loading Eo on tea stem porous carbon(BC@Eo),and their controlled-release fungicidal activity against Exobasidium vexans was assessed.BC with a large specific surface area of 1001.6 m2/g and mesoporous structure was fabricated through carbonization tempera-ture of 700℃.The BC@Eo materials were characterized using Fourier-transform infrared spectroscopy and X-ray powder diffraction.The results suggested that chemical and physical interactions occurred in BC@Eo.The Eo release profile suggested a biphasic pattern with an initial fast release on days 1–14 and a subsequent controlled phase on days 14–30.The in vitro cumulative release percentage of Eo from BC@Eo was 51%during one month,and this result was significantly lower than that from free Eo(cumulative release percentage of Eo of 82%in one week).The anti-fungal activities of Eo and BC@Eo against E.vexans were determined using the inhibition zone method.The results indicated that Eo and BC@Eo formed large inhibition zones of 19.66±0.79 and 21.92±0.77 mm,respectively.The influence on the hyphal structure of E.vexans was observed by scanning electron microscopy on day 30.The hyphal structure of E.vexans treated with BC@Eo was more shrunken than that treated with Eo at 30 days,suggesting that BC@Eo prolongs the fungicidal activity against E.vexans.This study demonstrated that the encapsulation of Eo in BC for developing the BC@Eo materials could be a promising strategy to inhibit volatility and maintain the fungicidal activity of Eo and provide a potential alternative for the reuse of abundant tea biomass waste resources.
基金supported by the Natural Science Fund for Distinguished Young Scholars of Tianjin (17JCJQJC45500)the National Natural Science Foundation of China (NSFC,21876091 and 22178181)Tianjin Municipal Science and Technology Project (18PTZWHZ00150).
文摘In-situ MgO-doped ordered mesoporous carbon(OMC@MgO)was fabricated by formaldehyde-free self-assembly method,in which biomass-derived tannin was used as carbon precursor replacing fossil-based phenolics,Mg^(2+)as both cross-linker and precursor of catalytic sites.Up to~20 wt% MgO could be doped in the carbon skeleton with good dispersion retaining well-ordered mesoporous structures,while more MgO content(35 wt%)led to the failing in the formation of ordered mesoporous structure.The OMC@MgO possessed a high specific surface area(298.8 m^(2) g^(-1)),uniform pore size distribution(4.8 nm)and small crystallite size of MgO(1.73 nm)due to the confinement effect of ordered mesoporous structure.Using OMC@MgO as the heterogeneous catalyst,a maximum fructose yield of 32.4% with a selectivity up to 81.1%was achieved from glucose in water(90℃,60 min),which is much higher than that obtained using the MgO doped active carbon via conventional post-impregnation method(26.5%yield with 58.3% selectivity).Higher reaction temperature(>90℃)resulted in decrease of selectivity due to the formation of humins.The designed OMC@MgO displayed tolerant to high initial glucose concentrations(10 wt%)and could remain good recyclability without significant loss of activity for three cycles.
基金financially supported by the National Natural Science Foundation of China (22008166)Natural Science Foundation of Shanxi (201901D211047)Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi (2019L0185)。
文摘Doping heteroatoms on carbon materials could bring some special advantages for using as catalyst support.In this work, a boron doped lamellar porous carbon(B-LPC) was prepared facilely and utilized as carbonbased support to construct Cu/B-LPC catalyst for dimethyl oxalate(DMO) hydrogenation. Doping boron could make the B-LPC own more defects on surface and bigger pore size than B-free LPC, which were beneficial to disperse and anchor Cu nanoparticles. Moreover, the interaction between Cu species and B-LPC could be strengthened by the doped B, which not only stabilized the Cu nanoparticles, but also tuned the valence of Cu species to maintain more Cu^(+). Therefore, the B-doped Cu/B-LPC catalyst exhibited stronger hydrogenation ability and obtained higher alcohols selectivity than Cu/LPC, as well as high stability without decrease of DMO conversion and ethylene glycol selectivity even after 300 h of reaction at 240℃.
基金the Science and Technology Research Project of Education Department of Jilin Province(JJKH20220683KJ)Natural Science Foundation of Jilin Province(20220101093JC).
文摘Common strategies for catalytic graphitization of biochar into graphitic porous carbon(GPC)still face great challenges,such as the realization of simple procedures,energy conservation,and green processes.Controlling over the graphitization degree and pore structure of biochar is the key to its structural diversification.Herein,a clean and energy-efficient method is developed to synthesize adjustable graphitic degree and structure porosity GPC from rice husk-based carbon(RHC)at a relatively low temperature of 800–1000°C with environment-benign organometallic catalyst ethylenediaminetetraacetic acid ferric sodium salt(EDTA-iron)and the recovery ratio of catalyst is as high as 97%.The formed by the organic ligands of EDTA-iron facilitates the etching of RHC surface and pore by iron,resulting in highly graphitized and developed porous GPCs.The pore structure and graphitization degree of GPCs can be adjusted by altering the catalyst loading,temperature,and holding time.The catalyst EDTA-iron with a lower concentration mainly plays the role of etching,which promotes the formation of porous carbon with larger surface area(SBET=1187.2 m^(2)·g^(-1)).The catalyst with higher concentration mainly plays the role of catalyzing graphitization and promotes the obtaining of graphitic carbon with high graphitization degree(ID/IG=0.19).The mechanism of EDTA-iron catalyzed graphitization of RHC is explored by the comprehensive analysis of BET,XRD,Raman,TEM and TGA.This research not only provides an efficient method for the preparation of high-quality biomass-based graphite carbon,but also provides a feasible method for the preparation of biomass-based porous carbon.
基金supported by the National Science Foundation of China(21805235)the Opening Foundation of Creative Platform of the Key Laboratory of the Education Department of Hunan Province(20K131)the Construct Program of the Key Discipline in Hunan Province。
文摘Rational design and exploration of low-cost and robust bifunctional oxygen electrocatalysts are vitally important for developing high-performance zinc-air batteries(ZABs).Herein,we reported a facile yet cost-efficient approach to construct a bifunctional oxygen reduction reaction(ORR)/oxygen evolution reaction(OER)electrocatalyst composed of N-doped porous carbon nanosheet flowers decorated with Fe Co nanoparticles(Fe Co/N-CF).Rational design of this catalyst is achieved by designing Schiff-base polymer with unique molecular structure via hydrogen bonding of cyanuramide and terephthalaldehyde polycondensate in the presence of metal cations.It exhibits excellent activity and stability for electrocatalysis of ORR/OER,enabling ZAB with a high peak power density of 172 m W cm^(-2)and a large specific capacity of 811 m A h g^(-1)Znat large current.The rechargeable ZAB demonstrates excellent durability for 1000 h with slight voltage decay,far outperforming a couple of precious Pt/Ir-based catalysts.Density functional theory(DFT)calculations reveal that high activity of bimetallic Fe Co stems from enhanced O_(2)and OH-adsorption and accelerated O_(2)dissociation by OAO bond activation.
基金the National Natural Science Foundation of China(NSFC)(Nos.12205100 and 11665017)the Key Scientific Research Project in Colleges and Universities of Henan Province,China(No.23B140002)the Key Project of College Students'Innovation and Entrepreneurship Training Program 2022 of North China University of Water Resources and Electric Power(No.2022XA050)。
文摘In order to deal with the increasingly serious environmental problems,it is important and necessary to lower the concentration of greenhouse gases,especially the CO_(2)gas.CO_(2)capture and storage are the relative suitable options for the reduction of these harmful gas concentration.Through the variation of mass ratio of KOH to bio-char,the as prepared active carbon PC-4 exhibits a higher specific surface area of 2491.57 cm^(3)·g^(−1),with the ultra-micropores of 0.5 and 1.2 nm.At 298 K/1 bar,the CO_(2)adsorption capacity of PC-4 also represents the highest value of 5.81 mmol/g.This work demonstrates that the both the pore size and the specific surface area are equally important to enhance the CO_(2)adsorption.This work provides a sustainable method to develop high efficiency waste-based adsorbents to deal with environmental issues of CO_(2)gas.
基金he Australian Research Council for financial support(ARC,DE190100965,FL190100126 and CE230100032).
文摘Continuous accumulation and emission into the atmosphere of anthropogenic carbon dioxide(CO_(2)),a major greenhouse gas,has been recognized as a primary contributor to climate change associated with the global warming and acidification of oceans.This has led to drastic changes in the natural ecosystem,and hence an unhealthy ecological environment for human society.Thus,the effective mitigation of the ever increasing CO_(2)emission has been recognized as the most important global challenge.To achieve zero carbon footprint,novel materials and approaches are required for potentially reducing the CO_(2)release,while our current fossil-fuel-based energy must be replaced by renewable energy free from emissions.In this paper,porous carbons with hierarchical pore structures are promising for CO_(2)adsorption and electrochemical CO_(2)reduction owing to their high specific surface area,excellent catalytic performance,low cost and long-term stability.Since efficient gas-phased(electro)catalysis involves the access of reactants to active sites at the gas-liquid-solid triple phase,the hierarchical porous carbon materials possess multiple advantages for various CO_(2)-related applications with enhanced volumetric and gravimetric activities(e.g.,CO_(2)uptake and current density)for practical operations.Recent studies have demonstrated that porous carbon materials exhibited notable activities as CO_(2)adsorbents and provided facile conducting pathways and mass diffusion channels for efficient electrochemical CO_(2)reduction even under the high current operation conditions.Herein,we summarize recent advances in porous carbon materials for CO_(2)capture,storage,and electrochemical conversion.Prospectives and challenges on the rational design of porous carbon materials for scalable and practical CO_(2)capture and conversion are also discussed.
基金financial support by the Foundation(No.GZKF202211)of State Key Laboratory of Biobased Material and Green Papermaking(Qilu University of Technology,Shandong Academy of Sciences)the Doctor of Suzhou University Scientific Research Foundation(2020BS015)+2 种基金Primary Research and Development Program of Anhui Province(201904a05020087)the Natural Science Research in Universities of Anhui Province in China(KJ2017A437,KJ2020A0727,KJ2020A0738 and KJ2020A0730,2022AH051363)the Provincial Natural Science Foundation of Anhui(1908085ME120).
文摘With the emergence of supercapacitors(SCs),the creation of bio-based electrode materials has grown in significance for the advancement of energy storage.However,it is particularly difficult for cathode materials to meet the demands of practical uses due to their low energy density.Herein,MIL-88 was fabricated in situ on the surface of cotton fibers used in cosmetics,followed by creating Fe_(2)N@porous carbon fiber composite(Fe_(2)N@PCF)through heat treatment at various temperatures.Fe_(2)N@PCF-800 demonstrates excellent specific capacitance performance(552 F g^(-1) at 1 A g^(-1)).Meanwhile,The AC//Fe_(2)N@PCF-800 device exhibits the largest energy density of 38 Wh kg^(-1) at 800 W kg^(-1) and a long cycling stability(83.3%capacity retention after 6000 cycles).Our elaborately designed Fe_(2)N@PCF demonstrate multiple advantages:i)the Fe_(2)N@PCF-800 shows abundant mesopores,providing abundant ion-diffusion pathways for mass transport and rich graphite microstructures,improving electrical conductivity for electron transferowning;ii)the rich nitrogen dopants and Fe_(2)N structure within all carbon components increase the capacitance through their pseudocapacitive contribution.These findings highlight the importance of biomass derived carbon materials for SCs applications.
基金Projects (51272221,51072173,21203161) supported by the National Natural Science Foundation of ChinaProject (10CY005) supported by Industrial Project of Colleges and Universities of Hunan Province,China
文摘The hierarchically porous carbons (HPCs) were prepared by sol-gel selassembly technology in different surfactant concentrations and were used as the potential electrode for lithium oxygen batteries. The physical and electrochemical properties of the as-prepared HPCs were investigated by filed emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), nitrogen adsorption-desorption isotherm and galvanostatic charge/discharge. The results indicate that all of the HPCs mainly possess mesoporous structure with nearly similar pore size distribution. Using the HPCs as the electrode, a high discharge capacity for lithium oxygen battery can be achieved, and the discharge capacity increases with the specific surface area. Especially, the HPCs-3 oxygen electrode with CTAB concentration of 0.27 mol/L exhibits good capacity retention through controlling discharge depth to 800 mA·h/g and the highest discharge capacity of 2050 mA·h/g at a rate of 0.1 mA/cm2.