SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Jing Ding,Chenhui Qiu,Zhiqiang Zhang,Qinghua Qu,Cheng Fang,Jinfeng Zhang,Guofeng Guan,Hui Wan
Manipulating the oxidation states of transition metals is an ideal solution to achieve selective generation of different products and copper is widely used in CO 2 photocatalytic reduction to methanol. However, the understanding on the effects of valence states of copper species in SrTiO 3 on its structure and the selectivity of the corresponding product in CO 2 photocatalysis are currently still limited. Here, copper-doped SrTiO 3 nanofibers with different controllable ratios of Cu + /Cu 2+ and Cu + /Cu 0 were prepared by the combination of the electrospinning with the in-situ reduction method. The proportion of copper with different valence states (Cu + /Cu 2+ and Cu + /Cu 0 ) was changed by rationally adjusting the time of hydrogen reduction. The presence of monovalent copper facilitated the generation of reactive intermediates, thereby enhancing its photocatalytic activity. The copper-doped SrTiO 3 nanofibers obtained after 3 h of hydrogen reduction (STCu 0.08 -H-3 h) had the highest proportion of Cu + /Cu 2+ and Cu + /Cu 0 with the highest methanol yield (6.96 μmol·g −1 ·h −1 ). Methanol generation rate and Cu + /Cu 2+ ratio of STCu 0.08 -H-xh (x = 1, 2, 3, 4,5) with different hydrogen reduction time were proven to be linearly positively correlated. Furthermore, theoretical investigation and in-situ CO 2 infrared spectrum deeply understood the difference of CO 2 adsorption behavior and CO 2 activation over Cu 2+ and Cu + of STCu 0.08 -H-3 h photocatalyst and the reaction intermediates involved in the photocatalytic CO 2 reduction to methanol.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Wei Shengjie,Zhu Jiexin,Chen Xingbao,Yang Rongyan,Gu Kailong,Li Lei,Chiang Ching-Yu,Mai Liqiang,Chen Shenghua
Breaking the geometric symmetry of traditional metal-N 4 sites and further boosting catalytic activity are significant but challenging. Herein, planar chlorination engineering is proposed for successfully converting the traditional Zn-N 4 site with low activity and selectivity for CO 2 reduction reaction (CO 2 RR) into highly active Zn-N 3 site with broken symmetry. The optimal catalyst Zn-SA/CNCl-1000 displays a highest faradaic efficiency for CO (FE CO ) around 97 ± 3% and good stability during 50 h test at high current density of 200 mA/cm 2 in zero-gap membrane electrode assembly (MEA) electrolyzer, with promising application in industrial catalysis. At -0.93 V vs. RHE, the partial current density of CO ( J CO ) and the turnover frequency (TOF) value catalyzed by Zn-SA/CNCl-1000 are 271.7 ± 1.4 mA/cm 2 and 29325 ± 151 h -1 , as high as 29 times and 83 times those of Zn-SA/CN-1000 without planar chlorination engineering. The in-situ extended X-ray absorption fine structure (EXAFS) measurements and density functional theory (DFT) calculation reveal the adjacent C-Cl bond induces the self-reconstruction of Zn-N 4 site into the highly active Zn-N 3 sites with broken symmetry, strengthening the adsorption of * COOH intermediate, and thus remarkably improving CO 2 RR activity.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Xinyi Jin,Laizhao Guo,Yangfeng Wang,Wentao Huang,Xiang Wang
Fruits are fragile and perishable during cold chain storage and transportation, leading to large economic losses. To cope with this problem, this study designs and develops a flexible gas sensing system to monitor the respiration rate of cold-chain fruits in real time, to warn of the decay process, and to help producers optimize their marketing and logistics strategies. The system consists of three parts: sensor, hardware circuit and host computer. The sensor responds to the carbon dioxide concentration in the microenvironment and outputs an initial electrical signal, which is collected and processed by the hardware circuit and then transmitted to the host computer via Bluetooth to output the final detection result. The core component is a flexible carbon dioxide sensor, which is made of flexible polyimide (PI) substrate, copper fork-finger electrode and polyethyleneimine-carbon nanotube (PEI-CNT) sensitive layer, and is prepared by laser printing and atomized spraying technology. The performance test results show that the sensor has high response rate, high sensitivity, good stability and flexibility, and can adapt to the cold chain low temperature environment. Through the performance test of the system, the results show that the system has a high accuracy, the absolute error is not more than 9%, and has good environmental adaptability, which can realize long-term stable work. In the experimental application for cold-chain kiwifruit, the system accomplished the real-time monitoring of carbon dioxide concentration changes, which verified its practical application performance in fruit quality monitoring. The system is designed to be lightweight and portable, with no mechanical damage to fruits, real-time monitoring and early warning capabilities, providing an effective solution for cold chain fruit quality monitoring.
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Molecular Catalysis
·
2025
·
IF 4.9
Liangliang Zhong,Wendong Wang,Hui Zheng,Xiaoyan Zeng,Fangsong Guo,Longmei Shang,Guowu Zhan
The electrochemical reduction of CO 2 (CO 2 RR) to formate is a promising strategy for carbon utilization and renewable energy storage. Herein, we develop a Cu 3 Bi 7 bimetallic nanosheet catalyst via an in situ topotactic transformation of BiOBr-CuBr heterojunctions. The resulting Cu 3 Bi 7 nanosheets feature abundant edge-active sites, enhanced electron transfer kinetics, and improved CO 2 adsorption, collectively boosting catalytic performance. Structural characterization confirms the coexistence of Cu and Bi phases in Cu 3 Bi 7 nanosheet, with strong electronic interactions optimizing the electronic structure, and mechanistic analysis indicates that the bimetallic synergy enhances CO 2 activation and stabilizes key intermediates, leading to superior selectivity and reaction kinetics. Electrochemical studies demonstrate that Cu 3 Bi 7 achieves a high formate Faradaic efficiency of 90 % at a current density of 120 mA cm -2 in a flow cell, maintaining exceptional stability for 90 h without performance degradation. This work provides a scalable strategy for designing efficient CuBi bimetallic catalysts and advances the development of CO 2 RR technology for practical applications.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lin Li,Kunpeng Yu,Jing Xie,Haixin Sun,Tong Feng,Qinqin Xu,Jianzhong Yin
Graphene has emerged as a highly promising material in the field of membrane separation due to its exceptional properties. However, the challenge of scalable production remains a significant barrier to its widespread application. In this study, we directly used graphene nanosheets (GNs) stripped by supercritical fluid as raw materials to prepare composite membranes with excellent performance. By systematically controlling the intercalation and phase-transition expansion of supercritical CO 2 under the guidance of the established exfoliation theory, a graphene dispersion with a concentration of 2.71 mg∙mL −1 was obtained, which is the highest value reported to date using the supercritical exfoliation (SCE) method. 90 % of the exfoliated GNs are <3 layers, 51 % of GNs exhibiting lateral dimensions >3 μm. The fabricated graphene composite membrane exhibited excellent dye rejection performance, achieving a rejection rate of 99.95 % for Congo red. This method addresses the limitations of conventional liquid-phase exfoliation methods, offering a scalable, cost-effective, and eco-friendly route for the production of graphene and related composite membranes.
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高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Xirui Yan,Haixia Liang,Ruicong Wang,Da Li,Jun Li,Wencai Peng,Jinli Zhang
CO 2 reforming with methane (DRM) is a potential effective carbon neutralization strategy to convert greenhouse gases into syngas. The key to the DRM process is to design active and coking resistant catalysts. Herein, hollow hierarchical bimetallic NiMo-HMgO catalysts were prepared via hydrothermal-impregnation method. The prepared NiMo-HMgO catalysts exhibited higher catalytic performance during the DRM process than commercial NiMo-CMgO catalysts, due to the formation of Ni-Mo-MgO composite on hierarchical MgO (HMgO), which is promoted by exposed (111) polar surface of HMgO with alternate arrangement of anion and cation layers. The deposited carbon and stability can be effectively regulated by adjusting the amount of Ni and the molar ratio of Mo/(Ni+Mo). The synergistic effect of metal and HMgO can provide reference for the research in other related fields.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Guangping Zhou,Hao Huang,Bo Yang,Xuan Zhou,Huoyan Jiang,Da Zhang,Wanli Zhang,Shaoqu Xie
A carbon-doped Cu/Al 2 O 3 catalyst was engineered using glucose, fructose, and sucrose as carbon sources. Controlled carbon deposition and calcination exposed acidic sites, thereby optimizing Cu dispersion, enhancing metal–support interaction (SMSI), and enriching surface hydroxyls, which collectively facilitated CO 2 hydrogenation via HCOO ∗ and ethyl acetate intermediates. Structural characterization showed that the preferential exposure of the Cu (111) crystal face further enhanced the catalytic activity. Performance tests showed that the catalyst exhibited a methanol yield of 12 % and a selectivity of 91 % in the CO 2 hydrogenation to methanol reaction, which was attributed to the improved Cu dispersion, the enriched metal Cu phase, and the presence of acidic sites. This study provides new ideas for the rational design of Cu-based catalysts and proposes a scalable green synthesis method for methanol.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Rui Xue,Shu Yuan,Rongyi Wang,Tianzi Bi,Guiru Zhang,Huiyuan Li,Jiewei Yin,Liuxuan Luo,Shuiyun Shen,Xiaohui Yan,Junliang Zhang
With the development of renewable energy, electrochemical carbon dioxide reduction reaction (CO 2 RR) has become a potential solution for achieving carbon neutrality. However, until now, due to issues with salt precipitate and regeneration of the electrolyte, this technology faces challenges such as difficulty in maintaining long-term stable operation and excessive costs. The pure water CO 2 electrolyzers are believed to be the ultimate solution to eliminate the salt depreciation and electrolyte issues. This study develops an in-situ method tailored for CO 2 reduction in pure water. By employing distribution of relaxation times (DRT) analysis and in-situ electrochemical active surface area (ECSA) measurements, we carried out a comprehensive investigation into the mass transport and electrochemical active surface area of gas diffusion electrodes (GDE) under pure water conditions. The maximum 89% CO selectivity and high selectivity (>80%) in the range of 0–300 mA/cm 2 were achieved using commercial Ag nanoparticles by rational design of catalyst layer. We found that ionomers influence the CO 2 electrolyzers performance via affecting local pH, GDE-membrane interface, and CO 2 transport, while catalyst loading mainly influences the active area and CO 2 transport. This work provides benchmark and insights for future pure water CO 2 electrolyzers development.
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高影响因子
CARBON
·
2025
·
IF 11.6
Lianzhong Shen,Lin Wang,Zhouwei Li,Yu Ye,Qizhou Dai
Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts are one of the more popular materials for electrochemical reduction of CO 2 to fuels and chemicals. Still, their Faraday efficiency and current density are generally low due to the single coordination environment and defect sites. Heteroatom doping has been demonstrated to increase the degree of defects in the material, improve the electron distribution at the single atomic sites, and enhance the catalytic performance. In this study, we prepared an S-doped single-atom catalyst called FeS@PC by a simple high-temperature pyrolysis method for efficient electroreduction of CO 2 to CO, with a maximum CO Faraday efficiency of 97.0% at -0.6 V vs. RHE potential. S atoms doped in the second-shell can change the electron distribution on the Fe-N 4 sites and accelerate the electron transfer during the electrochemical CO 2 reduction reaction (CO 2 RR). Through in situ ATR-FTIR characterization and kinetic experiments, it is found that the doped S can also promote the dissociation of H 2 O, provide sufficient protons for the conversion of CO 2 to *COOH, and promote the rate of CO conversion.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2016
·
IF 3.349
Zhihong Tian,Jiajia Huang,Zhonglu Zhang,Gonglei Shao,Ao Liu,Siguo Yuan
Novel Organic-inorganic hybrid microporous polymers with excellent thermal stability, high surface areas (1041 m 2 g −1 ) and controllable pore structures have been prepared via Scholl coupling and Friedel-Crafts reactions using Octaphenylcyclotetrasiloxane (OPCTS) as the building block, the pore structure of these OPCTS-based microporous polymers can be tuned by chosing crosslinking agent with different lengths of rigid connecting structure. Moreover, the as-prepared microporous polymers can serve as desirable carbon precursor to fabricate microporous carbons with uniform micromorphology, narrow pore size distribution , high microporosity (94%) and carbonization yield (58.8%). Both the hybrid microporous polymers and microporous carbons exhibit high CO2 adsorption capacities of 8.94 wt% (2.03 mmol g −1 ) and 14.78 wt% (3.36 mmol g −1 ) (273 K and 1 bar), respectively.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Weiyang Yuan,Shuzhen Chen,Changlei Qin,Dawid Piotr Hanak,Xu Zhou
CO2 adsorption is an important approach to control the excessive CO2 emission from energy and industrial plants and mitigating the greenhouse effect. As an acknowledged high-temperature adsorbent, Li4SiO4 shows advantages in capturing a large amount of CO2 with a fast reaction rate and excellent cyclic stability. However, its CO2 adsorption capacity would be significantly affected by the flue gas impurities, such as SO2 and O2. The underlying reaction mechanism of such impurities and Li4SiO4 is still unclear. For this reason, this work studied the reaction path and kinetics between Li4SiO4 and SO2 through experiments, thermodynamic calculations, and characterizations. The results showed that Li4SiO4 reacts with SO2 to produce Li2SiO3 and Li2SO4 in the presence of O2 at 500–700 °C and forms Li2SiO3 and Li2SO3 in the absence of O2 at 500–682 °C. Furthermore, this study revealed a very low activation energy of 7.47 kJ/mol for Li4SiO4 sulfation in the presence of O2 in the kinetic-controlled stage, and the value goes up to 249.7 kJ/mol in the diffusion-controlled stage. These results will provide valuable references for the industrial applications of CO2 adsorption by Li4SiO4.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2016
·Vol. 41
·期 1
·290-301
·
IF 3.277
Shokat Sarmad,Yujiao Xie,Jyri-Pekka Mikkola,Xiaoyan Ji
Deep eutectic solvents (DESs) as ionic liquid (IL) analogues show great potential for CO2 capture. They exhibit favorable solvent properties and are considered to be economical alternatives to conventional ILs. In this study, we prepare 35 DESs and screen them in terms of their CO2 solubility and viscosity, both crucial factors to be considered when designing efficient CO2 sorbents. The influence of salt and HBD type and structure, as well their molar ratio on the CO2 solubility and viscosity of the DESs is investigated. The viscosity and CO2 solubility of the DESs are compared with those of other DESs and conventional ILs. 15 DESs, which exhibit comparable CO2 absorption capacity to choline chloride–urea DESs, glycerol DESs and fluorinated ILs, are chosen as the promising ones. The viscosities of the selected DESs are below 200 mPa s and are lower than those of choline chloride-based DESs. Since the viscosity of the DESs is relatively high, on a par with those of conventional ILs, the effect of water as a co-solvent is investigated in order to decrease the viscosity. The addition of water to the glycerol-based DESs improves the kinetics of absorption by decreasing the viscosity, thus increasing the CO2 absorption capacity. Dry or aqueous DESs that demonstrate a high sorption capacity and low viscosity are chosen for additional analysis and characterization, and further functionalization will be carried out in the future to improve their sorption capacity.
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