ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Jianmin Wang,Ruoyu Huang,Haitao Huang,Haijin Li,Zhijie Chen,Jiajia Cai,Hao Zhang,Yongtao Li,Xiaofang Liu,Xiaolong Deng
Developing effective strategies to improve the electrocatalytic activity of carbon-based materials is significant for Zn-air batteries (ZABs). Herein, nitrogen-doped carbon with abundant sp3-hybridized carbon defects (NC-CTS) were synthesized through a nonthermodynamic equilibrium carbonization process called carbon thermal shock (CTS). The NC-CTS catalyst exhibited a superior oxygen reduction reaction (ORR) activity with a half-wave potential of 0.81 V vs RHE and good stability in alkaline electrolyte, exceeding the NC-Furnace catalyst, which was fabricated by a thermodynamic equilibrium process. The better ORR performance originated from the increased density of sp3-hybridized carbon defects as the active sites and the optimized adsorption energy of intermediate species. The sp3-hybridized carbon defects were attributed to the obstruction of atom mobility and aggregation due to the ultrashort duration time of CTS. Furthermore, the ZABs using NC-CTS catalysts as the cathode showed good discharge performance and high cycling stability with a power density of 110 mW cm–2. This study demonstrated an effective strategy to modulate the ratio of sp3/sp2 of carbon-based electrocatalysts for the development of advanced carbon-based electrocatalysts to enhance the ORR performance and for the development of ZABs.
研究领域:
材料科学
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电化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Peng Zhang,Cai Liang,Mudi Wu,Yongjie Li,Xiaoping Chen,Daoyin Liu,Jiliang Ma
The efficiency and sustainability for the recycling of plastic wastes into hydrogen was investigated. An integrated microwave-driven valorization of plastic wastes and CO 2 for H 2 and CO production was proposed. Specifically, plastic wastes were decomposed into H 2 and solid carbons, followed by carbon elimination via CO 2 gasification under microwave irradiation. Through the high-throughput screen of catalysts as well as the optimization of key parameters, over 96% hydrogen was converted into H 2 with a yield of 480 mmol∙g −1 H plastic while the carbon conversion and CO 2 conversion reached up to 70% and 53%. The five-cycle successive test displayed extraordinarily high and stable catalytic activity due to the facile elimination of carbon deposition. The application for real-world plastic wastes further demonstrated the efficient microwave-driven CO 2 gasification of plastic wastes into H 2 and CO production as a feasible and sustainable technology toward the waste-to-energy circular economy.
研究领域:
环境科学
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能源工程
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DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Shuang Gao,Xiuyan Deng,Xiaoming Qi,Hongbo Dai,Shao-Yun Fu,Yaqin Fu
High-performance microwave absorption materials with broad electromagnetic absorption bandwidths and scalable architectures have been increasingly demanded in modern electric and telecommunications industries. Herein, we propose a flexible three-dimensional (3D) woven fabric with superior washability and electromagnetic-wave absorption capability using the nanoengineered carbon black (CB)-Fe3O4/polyamide-66 (PA-66) composite fibers that possess a unique core–sheath structure. Notably, the impedance matching and microwave attenuation of the proposed 3D fabric absorbers are realized by the dielectric–magnetic coupling effect of nanometer-sized CB and Fe3O4 nanoparticles within the constituent PA-66 fibers. The produced 3D fabrics showed superior mechanical properties with a tensile strength of 35 MPa, good softness with flexibility of drape coefficient up to 88.8%, and great air permeability with an air permeability of over 109 mm/s. At a weft density of 250 picks/10 cm, the fabric realized the best electromagnetic-wave absorption performance with a minimum reflection loss of −34.5 dB, owing to the good impedance-matched 3D orthogonal structures and integrated dielectric–magnetic fibrous networks of the 3D fabric. In particular, this performance could be well-maintained even after rinsing five times or folding to two layers. This study can provide a promising route to developing next-generation flexible electromagnetic absorption materials.
研究领域:
材料科学
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电子工程
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DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2024
·
IF 5.9
Chengzhi Liu,Yanqi Zou,Kunmei Su,Zhenhuan Li
The emission of significant amounts of CO 2 from human industry has caused severe environmental damage, necessitating effective CO 2 capture methods for sustainable development. Membrane technology stands out as one of the most effective and economical solutions. In recent decades, polymer membranes have been recognized for their viability in gas separation applications. Aliphatic polycarbonates (APCs) are particularly notable due to their high chain segment flexibility, degradability, ease of processing, and the presence of carbonate groups, which enhance their affinity for CO 2 . This study uses a one-pot melt polycondensation process to synthesize three high-molecular-weight APCs: poly(1,4-butylene carbonate) (PBC), poly(1,5-pentamethylene carbonate) (PPC), and poly(1,6-hexamethylene carbonate) (PHC) from dimethyl carbonate and various diols. To improve the mechanical properties of the APC separation membranes, capping modification was applied. The molecular weights of PBC, PPC, and PHC were 6.48 × 10 4 g/mol, 4.78 × 10 4 g/mol, and 5.76 × 10 4 g/mol, respectively. These membranes were prepared by the evaporative solvent method. The PHC membrane demonstrated a CO 2 permeability of 20.84 Barrer and a CO 2 /N 2 selectivity of 22.24 at 35 °C under 0.1 MPa, approaching Robeson’s upper bound and indicating substantial potential for application.
研究领域:
材料科学
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环境工程
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化学工程
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DOI
高影响因子
ACS Catalysis
·
2025
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IF 13.1
Qianqian Song,Yingbing Zhang,Ziyang Wu,Min Kuang,Jun Chen,Jianping Yang
The electrocatalytic urea synthesis has emerged as a promising alternative strategy to replace the current energy-intensive industrial Haber–Bosch processes which are limited by sluggish C–N coupling and low selectivity because of the unmatched reduction kinetics of CO2 and nitrogen-based precursors. Herein, a thermodynamically spontaneous early stage C–N coupling pathway of *CO2 + *NO → *NOCO2 is established through the asymmetric bridging-adsorption of CO2 enabled by hydroxycarbonate-induced CO32–-Cu2+ dual sites on the tandem electrocatalyst of copper carbonate hydroxide and iron oxide grown on carbon fibers (CuCH/α-Fe2O3–CFs). This asymmetric adsorption induces a pronounced electron-deficient state of carbon atoms in CO2 due to bidirectional electron transfer toward both the CO32– and the Cu2+ centers. Coupled with the directional migration of *NO intermediates at the interface, effectively suppress the subsequent protonation of *CO2 while promoting nucleophilic attack by *NO, thereby driving spontaneous initial C–N coupling of *CO2 and *NO and significantly lowering the energy barrier of the C–N coupling step. The results demonstrate a urea Faradaic efficiency of 78.7% and urea yield rate of 1794.6 μg h–1 mgcat–1 at an ultralow applied potential of −0.20 V vs RHE, surpassing most reported catalysts to date.
研究领域:
电化学
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催化
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材料科学
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环境科学
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能量转换
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化学合成
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产品关联
DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Xuning Li,Yunpeng Li,Lin Wang,Jun Liu,Lin Chen,Xiao Zhu,Jingcheng Hao,Yongliang Ma,Junhua Li,Xu Wu
During thermal regeneration of styrene-saturated activated carbon (AC), styrene’s C=C bonds are prone to polycondensation. It forms fixed carbon species that deposit as carbonaceous residues within AC pores, significantly decreasing the adsorption performance. To address this challenge for efficient AC regeneration and recycling, Ni and Co transition metal components were loaded onto AC and subsequently pyrolyzed to generate NiCo2O4 active species. The optimal Ni–Co loading amount was determined to be 5 wt %. Under these conditions, the adsorbent exhibited optimal cyclic adsorption performance, maintaining 75% of its initial capacity after four consecutive adsorption–regeneration cycles. Comprehensive characterization revealed that the 2.5Ni-2.5Co-AC formulation maximized AC recyclability, and this enhanced performance is attributed to the well-dispersed NiCo2O4 species and the formation of carbon defect sites within the adsorbent. This study presents a novel strategy and provides a scientific basis for solving the regeneration problem of styrene-adsorbed activated carbon.
研究领域:
环境工程
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化学工程
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材料科学
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催化
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吸附技术
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产品关联
DOI
PubMed
高影响因子
FOOD HYDROCOLLOIDS
·
2022
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IF 11.504
Hao Zhang,Tuo Zhang,Jiachen Zang,Chenyan Lv,Guanghua Zhao
CO 2 is a greenhouse gas and a major contributor to global warming . Efficient conversion of CO 2 into high value-added food materials represents a promising strategy to decrease CO 2 concentration. In this study, we reported that Ca 2+ -crosslinked alginate beads loaded with carbonic anhydrase (CA) can efficiently catalyze conversion of CO 2 into porous vaterite CaCO 3 particles via a carboxymethyl cellulose (CMC) inducing process. CA encapsulated within the Ca 2+ -crosslinked alginate beads maintained around 100% activity of its original activity after 10 assay cycles. Functionally, the CA-loaded alginate beads facilitated conversion of CO 2 into porous vaterite CaCO 3 particles with high CO 2 removal efficiency in the presence of carboxymethyl cellulose. Notably, such vaterite CaCO 3 particles can be explored for adsorption of astaxanthin with higher loading capacity (2.0 wt %), consequently improving the photo- and thermal-stability of this pigment.
研究领域:
环境科学
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生物化学
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Biao Li,Yue Liu,Xiao Wu,Min Huang,Xiang Chen,Dong Huang,Chong Ye,Jianxiao Yang,Jinshui Liu,Ke Shen
Carbon-based insulation materials exhibit remarkable potential for use in thermal protection systems (TPS) in extreme environments such as hypersonic vehicles and deep-space missions. This is attributed to their ultralight structure, exceptional thermal insulation properties, and outstanding high-temperature stability. Nevertheless, traditional carbon aerogels frequently experience significant volume shrinkage during fabrication, which makes it challenging to optimize their structural and thermal performance. Inspired by the performance enhancement induced by hollow fiber structures, a carbide-derived carbon (CDC) strategy was employed in this study to fabricate a hollow carbon fiber-based porous insulation material (CF-H); carbon fiber felt (CF) was used as the structural template. The CDC strategy combined the template method with a conformal transformation mechanism to achieve minimal volume shrinkage (10.22%) and high porosity (98.84%). The hollow fiber framework reduced density (19 mg·cm −3 ), minimized heat transfer, and provided low thermal conductivity (0.09553 W·m −1 ·K −1 at 300 °C). Moreover, CF-H retained the needle-punched architecture of the CF template, thereby exhibiting excellent elasticity under mechanical stress. In conclusion, applying the CDC strategy to develop lightweight, high-performance carbon-based insulation materials offers a novel perspective on design and development of TPS insulation for application in extreme aerospace conditions.
研究领域:
材料科学
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航空航天工程
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yurui Xu,Xiao Liu,Minghui Jiang,Ning Li,Mingxue Su,Xin Du,Shiyu Li,Lei Lu,Suping Cui
Electrochemical carbon dioxide reduction reaction (ECO 2 RR) to produce high value-added products is a promising and effective strategy for closing the artificial carbon cycle and achieving sustainable development of resource. However, catalyst structural reorganization and agglomeration caused by the reduction process will reduce the catalytic performance. In this study, a carbon nitrogen shell with cupper-doped (CNCu shell) catalyst was prepared using silicon dioxide (SiO 2 ) as a template. The selectivity of the catalyst was controlled by precisely adjusting the form of Cu doping in the catalyst. When doped as single-atoms (CNCu 2.5 ), the catalyst exhibited a Faraday efficiency of up to 85 % for formate at −0.9 V versus reversible hydrogen electrode (vs. RHE). In contrast, when both Cu clusters and single-atoms coexisted (CNCu 25 ), the catalyst favored multi-carbon products, with a Faraday efficiency of 45 % for ethanol and 23 % for acetic acid. Density functional theory (DFT) calculations revealed the key mechanism for the difference in catalyst selectivity between the two doping forms. Cu single-atoms provided suitable binding energy to HCOO*, which increased the rate of CO 2 conversion to formate, while the combination of Cu clusters and single-atoms increased the adsorption of HCOO*, raising the rate-determining step energy of the formate pathway, which favored multi-carbon products. This study fundamentally revealed how different doping forms of metals affect catalyst selectivity, providing new insights and strategies for developing superior metal–carbon–nitrogen (M C N) catalysts.
研究领域:
电化学
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材料科学
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催化反应
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2023
·Vol. 170
·期 5
·053503
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IF 3.9
Tao Wu,Jintao Zhang,Yunfei Chen,Yongzheng Jia,Jialiang An,Jianbang Ge,Mingyong Wang
Molybdenum carbides are the promising ceramic materials and catalysts. A new and green method for the controllable preparation of molybdenum carbides was proposed by one-step co-electrolysis of Na2MoO4 and CO2 greenhouse gas in carbonate molten salts. The solubility and decomposition thermodynamics of Na2MoO4 were analyzed. The structure, composition, current efficiency, energy consumption and extraction ratio of molybdenum carbide were effectively regulated by changing the molten salt composition, electrolytic voltage, temperature, and electrolytic time. It was confirmed that MoC, Mo2C or dual-phase MoC-Mo2C can be controllably prepared. Molybdenum carbides may be mainly obtained by the thermal reaction between C from CO2 and Mo from Na2MoO4. Molybdenum carbides prepared at 850 °C and 4.5 V in Na2CO3-K2CO3−32 wt% Li2CO3−15 wt% Na2MoO4 molten salts showed the best electrocatalytic activity for hydrogen evolution reaction. The work provides an innovative and sustainable strategy to prepare molybdenum carbides and utilize CO2.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
高影响因子
RSC Advances
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2013
·Vol. 4
·期 5
·2360-2367
·
IF 2.562
Jin-Quan Wang,Wei-Guo Cheng,Jian Sun,Tian-Yuan Shi,Xiang-Ping Zhang,Suo-Jiang Zhang
Several novel 2-hydroxymethyl-functionalized ILs act as the catalysts for synthesis of cyclic carbonates from CO2 and epoxides without the use of any co-catalysts or organic solvent. Moreover, the 2-hydroxymethyl-functionalized ILs were compatible with base, which combined with K2CO3 were used as effective catalytic system for green synthesis of dimethyl carbonate from CO2via ethylene carbonate without catalyst separation. Additionally, the mechanistic details of the fixation of CO2 into cyclic carbonate catalyzed by 2-hydroxymethyl-functionalized ILs were also elucidated by density functional theory. The process reported here represents a simple, ecologically safer, cost-effective and energy-saving route to organic carbonates from CO2.
研究领域:
化学工程
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环境科学
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催化化学
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Feng Xie,Shaoqi Zhan,Zihan You,Jiao Lan,Linghu Meng,Wei Zheng,Yuanguo Chen,Ming Peng,Yongwen Tan
Electrochemical reduction of CO 2 , a technology with great potential for renewable energy storage and climate change mitigation, depends on critical C─C coupling steps in CO 2 RR to ensure efficient high-value hydrocarbon production. In this work, a local interface electric field and a tip-induced electric field are constructed on Ag-embedded Cu nanoneedle arrays to enhance the concentration of the *CO intermediate and regulate the adsorption of key intermediates, respectively. This optimization of the reaction microenvironment promotes the deep reduction of the *CO intermediate into multi-carbon products (C 2+ ), with a faradaic efficiency of 83.7% and a C 2+ local current density of −526 mA cm −2 within gas-fed flow cells. Experimental evidence and simulations validate that the interface electric field of the Cu-Ag bimetallic catalyst increased surface *CO coverage, substantially lowering the formation barrier for *CHO intermediate, and the tip-induced electric field that can stabilize *CO intermediate and suppress hydrogen evolution, promoting the C─C coupling process. The formation of the dual electric fields profoundly induced local environments and ultimately, the dominant C 2+ product, which offers significant design guidelines for adjusting the supply and demand balance of reaction intermediates.
研究领域:
电化学
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催化化学
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能源材料
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环境科学
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物理化学
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纳米材料
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可再生能源
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产品关联
DOI
高影响因子