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Fabricating sustainable lignin-derived porous carbon as electrode for high-performance supercapacitors

《化学科学与工程前沿（英文）》 2023年 第17卷 第8期   页码 1065-1074 doi: 10.1007/s11705-023-2313-0

摘要： Lignocellulosic biomass such as plants and agricultural waste are ideal to tackle the current energy crisis and energy-related environmental issues. Carbon-rich lignin is abundant in lignocellulosic biomass, whose high-value transformation and utilization has been the most urgent problem to be solved. Herein, we propose a method for the preparation of porous carbon from lignin employing an H3PO4-assisted hydrothermal method. We characterize the as-prepared lignin-derived porous carbon and investigate its potential for energy storage. After assisted hydrothermal treatment followed by carbonization at 800 °C, the lignin-derived porous carbon displays a high specific capacitance (223.6 F·g–1 at 0.1 A·g–1) and excellent cycling ability with good capacitance retention. In this present study, the resultant lignin-derived porous carbon was used as the electrode of a supercapacitor, illustrating yet another potential high-value use for lignin, namely as a candidate for the sustainable fabrication of main supercapacitor components.

关键词： lignin     porous carbon     electrode     supercapacitor    

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Hierarchically porous zeolites synthesized with carbon materials as templates

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1444-1461 doi: 10.1007/s11705-021-2090-6

摘要： Hierarchically porous zeolites are promising candidates in catalytic conversion of relatively bulky molecules, and their syntheses have attracted significant attention. From both industrial and scientific perspectives, different carbon materials have been widely employed as hard templates for the preparation of hierarchically porous zeolites during the past two decades. In this review, the progress in synthetic strategies using carbon materials as templates is comprehensively summarized. Depending on the affinity between the carbon templates and zeolite precursors, the substantial strategies for synthesizing hierarchical zeolites are introduced in direct templates and indirect templates. Direct templates methods, by which the carbon materials are directly mixed with precursors gel as hard templates, are first reviewed. Then, we discuss the indirect templates method (crystallization of carbon-silica composites), by which the carbon is produced by in situ pyrolysis of organic-inorganic precursors. In addition, the technique of encapsulating metal species into zeolites crystals with the assistance of carbon templates is also discussed. In the conclusion part, the factors affecting the synthesis of carbon-templated hierarchically porous zeolites are remarked. This review is expected to attract interest in the synthesis strategies of hierarchically porous zeolites, especially cost-effective and large-scale production methodologies, which are essential to the industrial application of hierarchical zeolites.

关键词： hierarchical zeolites     carbon materials     direct templates     indirect templates     carbon-silica composites    

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Boron and nitrogen co-doped porous carbon derived from sodium alginate enhanced capacitive deionization

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 2014-2024 doi: 10.1007/s11705-023-2346-4

摘要： Capacitive deionization can alleviate water shortage and water environmental pollution, but performances are greatly determined by the electrochemical and desalination properties of its electrode materials. In this work, B and N co-doped porous carbon with micro-mesoporous structures is derived from sodium alginate by a carbonization, activation, and hydrothermal doping process, which exhibits large specific surface area (2587 m2·g‒1) and high specific capacitance (190.7 F·g‒1) for adsorption of salt ions and heavy metal ions. Furthermore, the materials provide a desalination capacity of 26.9 mg·g−1 at 1.2 V in 500 mg·L‒1 NaCl solution as well as a high removal capacity (239.6 mg·g‒1) and adsorption rate (7.99 mg·g‒1·min‒1) for Pb2+ with an excellent cycle stability. This work can pave the way to design low-cost porous carbon with high-performances for removal of salt ions and heavy metal ions.

关键词： capacitance deionization     porous carbon     B/N co-doping     heavy metal ions     water purification    

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Single-Ni-atoms on nitrogenated humic acid based porous carbon for CO electroreduction

《化学科学与工程前沿（英文）》 2024年 第18卷 第5期 doi: 10.1007/s11705-024-2411-7

摘要： We proposed a facile synthesis of single-Ni-atom catalysts on low-cost porous carbon using a calcination method at the temperatures of 850–1000 °C, which were used for CO2 electrochemical reduction to CO. The porous carbon was prepared by carbonizing cheap and abundant humic acid. The structural characterizations of the as-synthesized catalysts and their electrocatalytic performances were analyzed. The results showed that the single-Ni-atom catalyst activated at 950 °C showed an optimum catalytic performance, and it reached a CO Faradaic efficiency of 91.9% with a CO partial current density of 6.9 mA·cm−2 at −0.9 V vs. reversible hydrogen electrode (RHE). Additionally, the CO Faradaic efficiency and current density of the optimum catalyst changed slightly after 8 h of continuous operation, suggesting that it possessed an excellent stability. The structure-activity relations indicate that the variation in the CO2 electrochemical reduction performance for the as-synthesized catalysts is ascribed to the combined effects of the increase in the content of pyrrolic N, the evaporation of Ni and N, the decrease in pore volume, and the change in graphitization degree.

关键词： CO2 electroreduction     single-Ni-atom catalysts     humic acid based porous carbon    

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High-yield production of porous carbon spheres derived from enzymatic hydrolysis lignin for zinc ion

《化学科学与工程前沿（英文）》 2024年 第18卷 第2期 doi: 10.1007/s11705-024-2387-3

摘要： The widespread implementation of supercapacitors is hindered by the limited energy density and the pricey porous carbon electrode materials. The cost of porous carbon is a significant factor in the overall cost of supercapacitors, therefore a high carbon yield could effectively mitigate the production cost of porous carbon. This study proposes a method to produce porous carbon spheres through a spray drying technique combined with a carbonization process, utilizing renewable enzymatic hydrolysis lignin as the carbon source and KOH as the activation agent. The purpose of this study is to examine the relationship between the quantity of activation agent and the development of morphology, pore structure, and specific surface area of the obtained porous carbon materials. We demonstrate that this approach significantly enhances the carbon yield of porous carbon, achieving a yield of 22% in contrast to the conventional carbonization-activation method (9%). The samples acquired through this method were found to contain a substantial amount of mesopores, with an average pore size of 1.59 to 1.85 nm and a mesopore ratio of 25.6%. Additionally, these samples showed high specific surface areas, ranging from 1051 to 1831 m2·g−1. Zinc ion hybrid capacitors with lignin-derived porous carbon cathode exhibited a high capacitance of 279 F·g−1 at 0.1 A·g−1 and an energy density of 99.1 Wh·kg−1 when the power density was 80 kW·kg−1. This research presents a novel approach for producing porous carbons with high yield through the utilization of a spray drying approach.

关键词： enzymatic hydrolysis lignin     porous carbon spheres     spray drying     zinc ion hybrid capacitors    

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Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1707-1717 doi: 10.1007/s11705-023-2308-x

摘要： Water electrolysis technology is considered to be one of the most promising means to produce hydrogen. Herein, aiming at the problems of high overpotential and slow kinetics in water splitting, N-doped porous carbon nanofibers-coupled CoNi2S4 nanoparticles are prepared as bifunctional electrocatalyst. In the strategy, NaCl is used as the template to prepare porous carbon nanofibers with a large surface area, and sulfur vacancies are created to modulate the electronic structure of CoNi2S4. Electron spin resonance confirms the formation of abundant sulfur vacancies, which largely reduce the bandgap of CoNi2S4 from 1.68 to 0.52 eV. The narrowed bandgap is conducive to the migration of valence electrons and decreases the charge transfer resistance for electrocatalytic reaction. Moreover, the uniform distribution of CoNi2S4 nanoparticles on carbon nanofibers can prevent the aggregation and facilitate the exposure of electrochemical active sites. Therefore, the composite catalyst exhibits low overpotentials of 340 mV@100 mA·cm–2 for oxygen evolution reaction and 380 mV@100 mA·cm–2 for hydrogen evolution reaction. The assembled electrolyzer requires 1.64 V to achieve 10 mA·cm–2 for overall water-splitting with good long-term stability. The excellent performance results from the synergistic effect of porous structures, sulfur deficiency, nitrogen doping, and the well-dispersed active component.

关键词： nanoparticle     sulfur vacancy     porous carbon nanofiber     transition metal sulfides     electrolysis    

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Synthesis of porous carbon from orange peel waste for effective volatile organic compounds adsorption

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 942-953 doi: 10.1007/s11705-022-2264-x

摘要： Volatile organic compounds have posed a serious threat to the environment and human health, which require urgent and effective removal. In recent years, the preparation of porous carbon from biomass waste for volatile organic compounds adsorption has attracted increasing attention as a very cost-effective and promising technology. In this study, porous carbon was synthesized from orange peel by urea-assisted hydrothermal carbonization and KOH activation. The role of typical components (cellulose, hemicellulose, and lignin) in pore development and volatile organic compounds adsorption was investigated. Among the three components, hemicellulose was the major contributor to high porosity and abundant micropores in porous carbon. Higher hemicellulose content led to more abundant –COOR, amine-N, and pyrrolic/pyridonic-N in the derived hydrochar, which were favorable for porosity formation during activation. In this case, the toluene adsorption capacity of the porous carbon improved from 382.8 to 485.3 mg·g–1. Unlike hemicellulose, cellulose reduced the >C=O, amine-N, and pyrrolic/pyridonic-N content of the hydrochar, which caused porosity deterioration and worse toluene adsorption performance. Lignin bestowed the hydrochar with slightly increased –COOR, pyrrolic/pyridonic-N, and graphitic-N, and reduced >C=O, resulting in comparatively poor porosity and more abundant micropores. In general, the obtained porous carbon possessed abundant micropores and high specific surface area, with the highest up to 2882 m2·g–1. This study can provide guidance for selecting suitable biomass waste to synthesize porous carbon with better porosity for efficient volatile organic compounds adsorption.

关键词： biomass waste     porous carbon     feedstock composition     urea-assisted hydrothermal carbonization     toluene adsorption     N-doped hydrochar    

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Cobalt-nitrogen co-doped porous carbon sphere as highly efficient catalyst for liquid-phase cyclohexane

《化学科学与工程前沿（英文）》 2024年 第18卷 第3期 doi: 10.1007/s11705-024-2395-3

摘要： The selective oxidation of cyclohexane to cyclohexanone and cyclohexanol (KA oil) is a challenging issue in the chemical industry. At present the industrial conversion of cyclohexane to cyclohexanone and cyclohexanol is normally controlled at less than 5% selectivity. Thus, the development of highly active and stable catalysts for the aerobic oxidation of cyclohexane is necessary to overcome this low-efficiency process. Therefore, we have developed a cobalt-nitrogen co-doped porous sphere catalyst, Co-NC-x (x is the Zn/Co molar ratio, where x = 0, 0.5, 1, 2, and 4) by pyrolyzing resorcinol-formaldehyde resin microspheres. It achieved 88.28% cyclohexanone and cyclohexanol selectivity and a cyclohexane conversion of 8.88% under Co-NC-2. The results showed that the introduction of zinc effectively alleviated the aggregation of Co nanoparticles and optimized the structural properties of the material. In addition, Co0 and pyridinic-N are proposed to be the possible active species, and their proportion efficiently increased in the presence of Zn2+ species. In this study, we developed a novel strategy to design highly active catalysts for cyclohexane oxidation.

关键词： KA oil production     cyclohexane selective oxidation     cobalt-nitrogen co-doped porous carbon spheres     metal-organic framework    

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Synthesis of micro/meso porous carbon for ultrahigh hydrogen adsorption using cross-linked polyaspartic

Jun Wei, Jianbo Zhao, Di Cai, Wenqiang Ren, Hui Cao, Tianwei Tan

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 857-867 doi: 10.1007/s11705-019-1880-6

摘要： In addition to the specific surface area, surface topography and characteristics such as the pore size, pore size distribution, and micro/mesopores ratio are factors that determine the performance of porous carbons (PCs) in the fields of energy, catalysis, and adsorption. Based on the mechanism of weight loss of polyaspartic acid at high temperatures, this study provided a new method for adjusting the surface morphology of PCs by changing the cross-linking ratio of the precursor, where cross-linked polyaspartic acid was used as precursor without additional activating agents. N adsorption analysis indicated that the specific surface area of the obtained PCs was as high as 1458 m ·g , of which 1200 m ·g was the contribution of the microporous area and the highest pore volume was 1.13 cm ·g , of which the micropore volume was 0.636 cm ·g . The thermogravimetric analysis results of the precursor, and also the scanning electron microscopy and Brunauer–Emmet–Teller analysis results of the carbonization product confirmed that the prepared PCs presented multilevel pore structure, and the diameters of most pores were 0.78 and 3.97 nm; moreover, the pore size distribution was relatively uniform. This conferred the PCs the ultrahigh hydrogen adsorption capacity of up to 4.52 wt-% at 77 K and 1.13 bar, in addition to their great energy storage and catalytic potential.

关键词： porous carbon     multilevel pores     polyaspartic acid     cross-linking     hydrogen adsorption    

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Concurrent adsorption and reduction of chromium(VI) to chromium(III) using nitrogen-doped porous carbon

《环境科学与工程前沿（英文）》 2022年 第16卷 第5期 doi: 10.1007/s11783-021-1491-6

摘要：

• A high-efficiency N-doped porous carbon adsorbent for Cr(VI) was synthesized.

关键词： Chromium(VI)     Nitrogen-doped porous carbon     Adsorption     Reduction     Loofah sponge    

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Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1289-1300 doi: 10.1007/s11705-023-2299-7

摘要： Environmental pollution caused by the presence of aromatic aldehydes and dyes in wastewater is a serious global concern. An effective strategy for the removal of these pollutants is their catalytic conversion, possibly to valuable compounds. Therefore, the design of efficient, stable and long-lifetime catalysts is a worthwhile research goal. Herein, we used nanofibrous carbon microspheres (NCM) derived from the carbohydrate chitin present in seafood waste, and characterized by interconnected nanofibrous networks and N/O-containing groups, as carriers for the manufacture of a highly dispersed, efficient and stable Pd nano-catalyst (mean diameter ca. 2.52 nm). Importantly, the carbonised chitin’s graphitized structure, defect presence and large surface area could promote the transport of electrons between NCM and Pd, thereby endowing NCM supported Pd catalyst with high catalytic activity. The NCM supported Pd catalyst was employed in the degradation of some representative dyes and the chemoselective hydrogenation of aromatic aldehydes; this species exhibited excellent catalytic activity and stability, as well as applicability to a broad range of aromatic aldehydes, suggesting its potential use in green industrial catalysis.

关键词： biowaste chitin     nanofibrous     palladium     nano-catalyst     catalysis    

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“Charging” the cigarette butt: heteroatomic porous carbon nanosheets with edge-induced topological defects

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1755-1764 doi: 10.1007/s11705-023-2318-8

摘要： Owing to the complexity of electron transfer pathways, the sluggish oxygen evolution reaction process is defined as the bottleneck for the practical application of Zn–air batteries. In this effort, metal nanoparticles (Co, Ni, Fe, etc.) encapsulated within nitrogen-doped carbon materials with abundant edge sites were synthesized by one-step pyrolysis treatment using cigarette butts as raw materials, which can drastically accelerate the overall rate of oxygen evolution reaction by facilitating the adsorption of oxygenated intermediates by the edge-induced topological defects. The prepared catalyst of nitrogen-doped carbon porous nanosheets loaded with Co nanoparticles (Co@NC-500) exhibits enhanced catalytic activity toward oxygen evolution reaction, with a low overpotential of 350 mV at the current density of 10 mA·cm–2. Furthermore, the Zn–air battery assembled with Co@NC-500 catalyst demonstrates a desirable performance affording an open-circuit potential of 1.336 V and power density of 33.6 mW·cm–2, indicating considerable practical application potential.

关键词： oxygen evolution reaction     porous carbon nanosheets     Co nanoparticles     edge-induced topological defects     Zn–air batteries    

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Enhancing comprehension of water vapor on adsorption performance of VOC on porous carbon materials and

《环境科学与工程前沿（英文）》 doi: 10.1007/s11783-024-1870-x

摘要：

● Water vapor’s effect on VOC adsorption in various porous carbons was investigated.

关键词： Adsorption     Water vapor     Carbon-based adsorbents     Surface functional groups     VOC properties    

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Electrospun porous carbon nanofibers derived from bio-based phenolic resins as free-standing electrodes

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 504-515 doi: 10.1007/s11705-022-2260-1

摘要： Phenolic resins were employed to prepare electrospun porous carbon nanofibers with a high specific surface area as free-standing electrodes for high-performance supercapacitors. However, the sustainable development of conventional phenolic resin has been challenged by petroleum-based phenol and formaldehyde. Lignin with abundant phenolic hydroxyl groups is the main non-petroleum resource that can provide renewable aromatic compounds. Hence, lignin, phenol, and furfural were used to synthesize bio-based phenolic resins, and the activated carbon nanofibers were obtained by electrospinning and one-step carbonization activation. Fourier transform infrared and differential scanning calorimetry were used to characterize the structural and thermal properties. The results reveal that the apparent activation energy of the curing reaction is 89.21 kJ·mol–1 and the reaction order is 0.78. The activated carbon nanofibers show a uniform diameter, specific surface area up to 1100 m2·g–1, and total pore volume of 0.62 cm3·g–1. The electrode demonstrates a specific capacitance of 238 F·g–1 (0.1 A·g–1) and good rate capability. The symmetric supercapacitor yields a high energy density of 26.39 W·h·kg–1 at 100 W·kg–1 and an excellent capacitance retention of 98% after 10000 cycles. These results confirm that the activated carbon nanofiber from bio-based phenolic resins can be applied as electrode material for high-performance supercapacitors.

关键词： lignin     bio-based phenolic resins     electrospinning     activated carbon nanofibers     supercapacitors    

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Carbon-doped surface unsaturated sulfur enriched CoS@rGO aerogel pseudocapacitive anode and biomass-derivedporous carbon cathode for advanced lithium-ion capacitors

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1500-1513 doi: 10.1007/s11705-021-2086-2

摘要： As a hybrid energy storage device of lithium-ion batteries and supercapacitors, lithium-ion capacitors have the potential to meet the demanding needs of energy storage equipment with both high power and energy density. In this work, to solve the obstacle to the application of lithium-ion capacitors, that is, the balancing problem of the electrodes kinetic and capacity, two electrodes are designed and adequately matched. For the anode, we introduced in situ carbon-doped and surface-enriched unsaturated sulfur into the graphene conductive network to prepare transition metal sulfides, which enhances the performance with a faster lithium-ion diffusion and dominant pseudocapacitive energy storage. Therefore, the lithium-ion capacitors anode material delivers a remarkable capacity of 810 mAh∙g–1 after 500 cycles at 1 A∙g–1. On the other hand, the biomass-derived porous carbon as the cathode also displays a superior capacity of 114.2 mAh∙g–1 at 0.1 A∙g–1. Benefitting from the appropriate balance of kinetic and capacity between two electrodes, the lithium-ion capacitors exhibits superior electrochemical performance. The assembled lithium-ion capacitors demonstrate a high energy density of 132.9 Wh∙kg–1 at the power density of 265 W∙kg–1, and 50.0 Wh∙kg–1 even at 26.5 kW∙kg–1. After 10000 cycles at 1 A∙g–1, lithium-ion capacitors still demonstrate the high energy density retention of 81.5%.

关键词： in-situ carbon-doped     surface unsaturated sulfur enriched     pseudocapacitive energy storage     biomass-derived carbon     lithium-ion capacitors    

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标题 作者 时间 类型 操作

Fabricating sustainable lignin-derived porous carbon as electrode for high-performance supercapacitors

期刊论文

Hierarchically porous zeolites synthesized with carbon materials as templates

期刊论文

Boron and nitrogen co-doped porous carbon derived from sodium alginate enhanced capacitive deionization

期刊论文

Single-Ni-atoms on nitrogenated humic acid based porous carbon for CO electroreduction

期刊论文

High-yield production of porous carbon spheres derived from enzymatic hydrolysis lignin for zinc ion

期刊论文

Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional

期刊论文

Synthesis of porous carbon from orange peel waste for effective volatile organic compounds adsorption

期刊论文

Cobalt-nitrogen co-doped porous carbon sphere as highly efficient catalyst for liquid-phase cyclohexane

期刊论文

Synthesis of micro/meso porous carbon for ultrahigh hydrogen adsorption using cross-linked polyaspartic

Jun Wei, Jianbo Zhao, Di Cai, Wenqiang Ren, Hui Cao, Tianwei Tan

期刊论文

Concurrent adsorption and reduction of chromium(VI) to chromium(III) using nitrogen-doped porous carbon

期刊论文

Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

期刊论文

“Charging” the cigarette butt: heteroatomic porous carbon nanosheets with edge-induced topological defects

期刊论文

Enhancing comprehension of water vapor on adsorption performance of VOC on porous carbon materials and

期刊论文

Electrospun porous carbon nanofibers derived from bio-based phenolic resins as free-standing electrodes

期刊论文

Carbon-doped surface unsaturated sulfur enriched CoS@rGO aerogel pseudocapacitive anode and biomass-derivedporous carbon cathode for advanced lithium-ion capacitors

期刊论文