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MICROPOROUS AND MESOPOROUS MATERIALS · 2024 · IF 4.8

Oriented construction of lignin-derived carbon hybrid electrocatalyst with superwettable surface and Co-based heterostructure for overall water splitting

Guoning Li,Yu Zhang,Weiyang Ma,Faming Liu,Hui Li

Converting lignin waste into carbon hybrid catalysts for water electrolysis engenders a beneficial scenario for both the valorization of waste carbon resources and the reduction of hydrogen production costs, which remains a grand challenge. Hence, we report a novel lignin-derived carbon hybrid electrocatalyst as a low-cost and highly efficient bifunctional electrocatalyst for overall water splitting, prepared by a feasible strategy involving NaCl-assisted pyrolysis and subsequent oxidation-phosphorization. Notably, this strategy can not only regulate the composition of CoP/CoO x nano-heterostructures but also improve the structural properties of porous carbon matrix. Profiting from superwettable surface, ultrafine Co-based heterojunctions and large active area, the optimal CoP/CoO x -HPC catalyst exhibits exceptional bifunctional catalytic activity in 1 M KOH electrolyte, requiring only small overpotentials of 396 and 522 mV for HER and OER, respectively, to achieve a large current density of 400 mA cm −2 . Meanwhile, the assembled alkali-electrolyzer using CoP/CoO x -HPC as both cathode and anode needs a relatively low voltage of 2.31 V at 400 mA cm −2 , significantly outperforming the commercial couple of Pt/C || RuO 2 . This work can be of value in the design of the low-cost and highly active lignin-derived electrocatalysts and also serve as guidance for the high-value utilization of lignin or even other biomass wastes.

CAS / MDL: 9005-53-2
研究领域: 材料科学 · 能源化学
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CATALYSIS TODAY · 2018 · IF 4.667

Esterification of oleic acid to biodiesel catalyzed by a highly acidic carbonaceous catalyst

Yi-Tong Wang,Zhen Fang,Fan Zhang

Carbonaceous catalyst, with a variety of acid sites, was successfully synthesized by a two-step method at low temperature. The synthesized catalyst (Zr-SO 3 H@CMC) was characterized by elemental analysis, XRD, ICP-OES, FT-IR, BET, SEM-EDX and Boehm titration. It had high total acid content (8.45 mmol/g) for oleic acid esterification with high biodiesel yields (> 99%) at 40–90 °C. Under conditions of 90 °C, 20/1 methanol/oleic acid molar ratio, 5 wt% catalyst and 2 h reaction time, biodiesel yield of > 87% was achieved after 10 cycles of use. At lower temperatures (40, 50 and 60 °C), biodiesel yield still reached 82%, 93% and 90% after 3 cycles, respectively. The high activity of Zr-SO 3 H@CMC benefited from low activation energy of 24.7 KJ/mol. It shows potential application for esterification of free fatty acids or pretreatment of oils with high acid value for the green production of biodiesel.

研究领域: 化学工程 · 可再生能源 · 催化科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Carbon monolith supported Fe-Based catalyst Boosts olefins production performance of Fischer-Tropsch synthesis via enhanced Mass-Transfer effect

Yang Wang,Ruosong He,Kaixuan Huo,Pei Dong,Xiaoli Fu,Shujie Sun,Feng Qiu,Yiwu Lu,Qiang Liu,Guangbo Liu,Noritatsu Tsubaki,Mingbo Wu

Even though the carbon-based Fischer-Tropsch synthesis (FTS) catalysts deliver excellent performance owing to the outstanding physicochemical property of carbon materials, the poor mechanical strength and difficulty in formability are the bottlenecks for their practical and industrial applications, especially in a fixed-bed reactor. To tackle this obstacle, we propose a stepwise heat treatment protocol to successfully fabricate a biomass-derived monolithic carbon material with favorable mechanical strength. The carbon monolith can be employed as promising Fe-based active sites carrier to boost the olefins production performance of FTS. Compared with the powdered counterpart under the same reaction conditions (260 °C, 3 MPa, CO:H 2  = 1:2, GHSV = 3000 mL g cat −1 h −1 ), the catalytic activity of the monolithic catalyst is significantly increased from 37.2 % to 64.3 % while maintaining the high selectivity of olefin products (68.1 %), therefore the maximum olefin space–time yield approaching to extremely high value of 666 mg g Fe3O4 -1 h −1 (260 °C, 3 MPa, CO:H 2  = 1:2, GHSV = 6000 mL g cat −1 h −1 ). Multiple characterizations reveal that the formation of interconnected monolithic structure can be attributed to the dehydration-polymerization reaction between the biomass carbon and binder. Based on the heat and mass transfer simulations, it is obvious that the monolithic catalyst possesses superior mass and heat transfer performance and better reactants diffusion behaviors, which contribute to the formation of more χ-Fe 5 C 2 active phase for C-O bond activation and C-C bond coupling. This work will shed new light on the rational design of highly efficient monolithic FTS catalyst with remarkable strength for practical application at large scale.

研究领域: 化学工程 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Decomposition of carbon-based catalysts in advanced oxidation processes: A neglected but noteworthy problem

Shizong Wang,Jianlong Wang

Carbon-based catalysts have been widely investigated in the field of advanced oxidation processes (AOPs), however their structural stability during the AOPs has been neglected. In this study, the decomposition of different carbonaceous materials, including g-C 3 N 4 , biochar, biochar/g-C 3 N 4 composite, graphene oxide and COF in sulfate radical-based and hydroxyl radical-based AOPs was investigated, mainly focusing on g-C 3 N 4 and modified g-C 3 N 4 in peroxymonosulfate (PMS)-based AOPs. The g-C 3 N 4 prepared with different precursors and modified g-C 3 N 4 were selected to investigate their structural stability in PMS-based AOPs in detail. The results showed that both g-C 3 N 4 and modified g-C 3 N 4 were partially decomposed in the PMS-based AOPs leading to the carbon dissolution in solution. The concentration of dissolved carbon varied with the precursor of g-C 3 N 4 and experimental conditions such as PMS concentration and inorganic ions. Modified g-C 3 N 4 presented higher concentration of dissolved carbon than pristine g-C 3 N 4 . Based on the results of experiments and characterization, the decomposition of g-C 3 N 4 and modified g-C 3 N 4 were mainly due to their interaction with PMS. Modified g-C 3 N 4 had higher adsorption capacity for PMS than pristine g-C 3 N 4 leading to the enhanced interaction with PMS. The dissolved carbon from modified g-C 3 N 4 would not affect the removal efficiency, but the mineralization efficiency of targeted organic pollutants. In addition, the dissolved components of g-C 3 N 4 and modified g-C 3 N 4 showed acute toxicity. In addition to g-C 3 N 4 -based catalysts, other materials such as covalent organic compound and graphene oxide could be also decomposed partially. The decomposition of g-C 3 N 4 was also found in the peroxydisulfate and hydrogen peroxide-based AOPs. This study provided insight into the structural stability of g-C 3 N 4 -based catalysts in the PMS-based AOPs, which deserved much attention in the future studies from the point view of the design and environmental application of g-C 3 N 4 -based catalysts.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Synthesis of tung oil-based polyphenols via phosphotungstic acid loaded tung meal-based carbon-catalyzed Friedel-Crafts alkylation: A smart way to access renewable bio-based polyurethanes

Baozheng Zhao,Fei Song,Qi Zhao,Zheng Pan,Yijiao Xue,Guodong Feng,Meng Zhang,Yonghong Zhou

Achieving green preparation and economical recycling of polyurethane (PU) foams while considering environmental protection and comprehensive resource utilization is a significant challenge. Herein, we have proposed an integrated utilization strategy of tung oil fruit to design tung oil-based PU (TPU) foams with malleability and thermal processability. Phosphotungstic acid was first loaded onto tung meal-based carbon derived from the solid microwave carbonization of waste tung meal to obtain carbon-based catalysts with a total acid density of up to 2408.4 μmol/g. In the Friedel-Crafts alkylation reaction of tung oil and guaiacol, the carbon-based catalysts show highly catalytic performance and reusability, resulting in the phenolic hydroxyl content of tung oil-based polyphenols reaching 3.05 mmol/g. The TPU foams containing phenol-carbamate bonds were prepared from tung oil-based polyphenols, which can be processed into TPU films through thermal compression molding. The recycled TPU films show tunable mechanical properties and can be further reprocessed. We have also produced carbon fiber-reinforced composites with TPU as the matrix, which have good mechanical properties and can be sustainably recycled. This research aims to produce closed-loop recycling-oriented TPU foams using forest resources as raw materials while adequately using waste to achieve green production processes.

CAS / MDL: 98-94-2 111-65-9
研究领域: 材料科学 · 绿色化学 · 林产化学加工
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FUEL PROCESSING TECHNOLOGY · 2022 · IF 8.129

Microwave-assisted catalytic alcoholysis of fructose to ethoxymethylfurfural (EMF) over carbon-based microwave-responsive catalyst

Xiaowen Ge,Hong Li,Mengyuan Liu,Zhenyu Zhao,Xin Jin,Xiaolei Fan,Xin Gao

Ethoxymethylfurfural (EMF) is a promising fuel additive and biofuel which can be produced via catalytic direct alcoholysis of fructose. In this work, microwave-responsive catalysts were prepared by carbonization of cellulose (via either hydrothermal treatment or calcination) then functionalized with SO 3 H group (via impregnation using concentrated sulfuric acid), which exhibit remarkable performances in one-pot catalytic conversion of fructose to EMF with ethanol. After a 8 h reaction under microwave irradiation at 75 °C, about 80.3% fructose conversion was achieved with the EMF yield of 61.2% for the carbon catalyst prepared by the hydrothermal treatment, which is much higher than that achieved by the catalysis promoted by conventional heating. Further investigation showed that with a microwave-responding catalyst, microwave irradiation encourages the formation of local hot-spots on the catalyst surface, thus facilitating the collision of reactant molecules with catalysts to improve the catalytic efficiency. This work demonstrates the potential of microwave-responsive heterogeneous catalysts for process intensification of valorization of bio-derived chemicals under microwave irradiation.

研究领域: 化学工程 · 可再生能源
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Catalysts · 2023 ·Vol. 13 ·期 9 ·1307 · IF 3.9

Sterical Self-Consistency of Carbonaceous Nanopolyhedra Triggered by Introduced CNTs to Optimize ORR Performance

Yuanhui Zuo,Yanlong Tang,Huancong Shi,Shijian Lu,Paitoon Tontiwachwuthikul

The electrocatalyst of oxygen reduction reactions is one of the basic components of a fuel cell. In addition to costly Pt/C benchmark catalysts, cost-effective carbon-based catalysts have received the most attention. Enormous efforts have been dedicated to trade off the catalyst performance against the economic benefit. Optimizing composition and/or structure is a universal strategy for improving performance, but it is typically limited by tedious synthesis steps. Herein, we have found that directly introducing CNT into MOF-derived carbonaceous nanopolyhedra, i.e., introduced carbon nanotubes (CNTs) penetrated porous nitrogen-doped carbon polyhedra (NCP) dotted with cobalt nanoparticles (denoted as CNTs-Co@NCP), can optimize the catalytic activity, stability, and methanol tolerance. The hierarchical architecture combines the 0D/1D/3D Co/CNT/NCP interfaces and 1D/3D CNT/NCP junctions with the frameworks with a greatly exposed active surface, strengthened mass transport kinetics, stereoscopic electrical conductivity networks and structural robustness. The sterical self-consistency of MOF-self-assembly triggered by introduced CNTs demonstrates tactful ORR electrocatalytic activity regulation. Eventually, the CNTs-Co@NCP showed a half-wave potential (E1/2) of 0.86 V and a diffusion-limited current density (JL) of 5.94 mA/cm2in alkaline electrolyte. The CNTs-Co@NCP was integrated into the cathode of a direct methanol fuel cell (DMFC) with an anion-exchange membrane, and an open-circuit voltage (OCV) of 0.93 V and a high power density of 46.6 mW cm−2were achieved. This work successfully developed a catalyst with competitive ORR performance through plain parameter fine-tuning without complex material design.Keywords:oxygen reduction reaction;sterical self-consistency;carbon-based catalyst;stereoscopic conductive network;DMFC

研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Phosphor-doping modulates the d-band center of Fe atoms in Fe-N4 catalytic sites to boost the activity of oxygen reduction

Yuan Qin,Zihao Ou,Chaozhong Guo,Yao Liu,Rong Jin,Chuanlan Xu,Haifeng Chen,Yujun Si,Honglin Li

Regulating the electronic structure by phosphor-doping is a preferred strategy to boost the performance of carbon-based catalysts for oxygen reduction reaction (ORR). Here, a porous Fe, P, N-codoped carbon catalyst (PCF-FeTz-900) is designed by a phytic acid-assisted thermal etching strategy, in which P atoms are first doped into the carbon matrix to form a stable P C bond, and then FeN 4 sites are produced from Fe-2,4,6-Tris(2-pyridyl)-s-triazine complex (Fe-TPTz). Theoretical calculations suggest that the electrons are transferred from the doped P atom to the neighboring FeN 4 sites, which facilitates the ORR at the Fe sites by reducing the energy barrier and the adsorption energy of intermediates. Additionally, the P-doped FeN 4 (FeN 4 P) structure manifests a lower free energy difference than that of FeN 4 and the d -band center of Fe is also lowered, which further ensures its higher ORR catalytic ability. As a result, the PCF-FeTz-900 catalyst exhibits superior ORR activity and stability in alkaline electrolyte, and the assembled primary zinc-air battery shows greater performances compared to the commercial Pt/C catalyst. This work can provide an effective pathway for modulating the performance of doped-carbon materials in energy conversion devices.

研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Construction of MnX (X = P, O, S) nanoparticles embedded in porous carbon/graphene nanocomposite fibers as efficient bifunctional oxygen electrocatalyst for Zn–air batteries

Siyuan Sun,Xiaoyun Zhang,Yang Sun,Fan Yang,Tianyu Bai,Cunhui Yu,Kexin Wei,Haojia Zhong,Qiang Wei,Yongfeng Li

Porous carbon coated manganese compounds nanoparticles (MnX, X = P, O or S) is a kind of potential catalysts for oxygen electrocatalysis due to the controllable d-band center, while the complex mechanism and performance difference is yet to reveal due to the lack of catalyst platform. Herein, the ORR catalytic activity and difference reason between manganese phosphide, oxide, and sulfide are tested and discussed via manganese compounds contained carbon-based catalyst platforms synthesis and Density functional theory (DFT). Manganese compounds nanoparticles active sites are uniformly distributed in porous carbon fibers/graphene composite, which guarantees the high mass transfer ability and conductive ability. Experiment results show that catalyst with Mn 2 P active sites exhibits best bifunctional catalytic activity for ORR/OER, which only need 0.89 V (vs. RHE) to achieve a half-wave potential (E 1/2 ) in ORR and 1.58 V (vs. RHE) to reach the overpotential at 10 mA cm −2 (E 10 ) in OER. Theoretical analysis shows that the d-band center of Mn in Mn 2 P is much closer to the Fermi level than MnS and MnO. The rate-determining process of Mn 2 P has the smallest energy barrier of 0.56 eV, indicating the best ORR activity. This work provides paves a solid way for the synthesis of carbon-based catalysts with manganese compounds active sites.

CAS / MDL: 13446-34-9 83-86-3
研究领域: 材料科学 · 电化学
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Plasma Processes and Polymers · 2024 · IF 2.9

Ni-MOF-74 Derived Carbon-Based Ni Catalysts for Efficient Catalytic Ammonia Synthesis via Pulsed DBD Plasma

Qinlong Song,Xianyi Yin,Haibao Zhang

Designing efficient noble metal-free catalysts for plasma-catalytic ammonia synthesis is significant and challenging. Carbon-based metal catalysts were prepared at different pyrolysis temperatures using the Ni-MOF-74 precursor. The effects of Ni-MOF-74 and its derived carbon-based metal catalysts on pulsed dielectric barrier discharge (DBD) plasma ammonia synthesis were investigated. The results showed that Ni-MOF-74-300 with both the MOF structure and nickel metal particles exhibited the best catalytic performance for ammonia synthesis. The ammonia synthesis rate reached 41.38 mmol g −1 h −1 , whereas the nitrogen conversion rate was as high as 1.54% with an energy yield of 3.04 g kWh −1 . Compared to the situation of plasma only, the ammonia synthesis rate, nitrogen conversion rate, and energy yield were increased by 28.46 times, 5.7 times, and 5.5 times, respectively.

研究领域: 化学工程 · 催化材料科学
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NEW JOURNAL OF CHEMISTRY · 2017 ·Vol. 41 ·期 12 ·4959-4965 · IF 3.269

A hybrid composite catalyst of Fe3O4 nanoparticles-based carbon for electrochemical reduction of oxygen

Zongkun Chen,Fei Lin,Dandan He,Heqing Jiang,Jingjing Zhang,Xin Wang,Minghua Huang

The design of efficient and cheap electrocatalysts for the oxygen reduction reaction (ORR) plays a key role for renewable energy technologies such as fuel cells and metal–air batteries. Using a simple and effective route, electronically conductive acetylene black (AB) was deliberately introduced into Fe3O4/HCS-600 with enough ORR active sites to be used as an ORR catalyst. The good homogenization of the electron conductor AB and the high intimate contact of Fe3O4/HCS-600 and AB in the composite catalyst provide the possibility of facile electron accessibility. The resulting composite catalyst exhibited a high and stable electrocatalytic activity for the ORR, which is better than Fe3O4/HCS-600 or AB alone. These features may offer potential for the development of efficient ORR catalysts with low cost for alkaline fuel cells.

研究领域: 材料科学 · 能源技术 · 电化学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Endogenous calcium enriched hydrochar catalyst derived from water hyacinth for glucose isomerization

Luhan Yang,E. Shuang,Jianglong Liu,Kuichuan Sheng,Ximing Zhang

Water hyacinth is a major aquatic plant in ecological restoration which propagates rapidly, whereas its biomass waste lacks value-added utilization routes. To address this problem, we put forth an innovative two-step carbonization strategy to convert water hyacinth to catalyst for isomerization of glucose to fructose. Through combining the hydrothermal carbonization and pyrolysis , catalyst morphology including its carbon substrate and calcium salts was successfully engineered. The prepared hydrochar-based catalyst presented an outstanding catalytic performance, the optimal of which could obtain 31% fructose yield with 89% selectivity at 120 °C for 45 min in water and maintain the reactivity for at least three runs. The catalytic reactivity was derived from the crystallization of endogenous alkaline earth calcium in water hyacinth, which was comparable to catalysts doped with expensive metals. Besides, the equipment and energy requirements for preparation were quite low-demanding (calcined only at 400 °C for 1 h). This study not only pioneers a sustainable way to upcycle aquatic biomass, but also invents a low-cost and efficient catalyst for biorefinery through the production of engineered carbon.

CAS / MDL: 57-48-7 50-99-7 57-13-6
研究领域: 环境科学 · 生物化学 · 催化材料
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