Science China-Materials
·
2024
·Vol. 67
·期 3
·788-795
·
IF 6.8
Song Dewen,Zhang Shipeng,Ning Hui,Fei Xiang,Wang Mingwang,Wang Xiaoshan,Wu Wenting,Zhao Qingshan,Li Yongzhe,Wu Mingbo
CO 2 electroreduction is an alluring technology for high-value CO 2 utilization and intermittent electrical energy storage. Self-supporting catalysts with high efficiency have clear advantages over powder ones in electrode construction but still lack effective synthesis methods. In this work, a self-supporting BiCu/carbon hybrid nanofiber membrane (BiCu/CHNM) was synthesized by electrospinning-calcination and employed directly as a working electrode in a flow cell for CO 2 electroreduction to formate with a high Faradaic efficiency of 87.67% at a partial current density of 142.9 mA cm −2 . In stability tests, the Faradaic efficiency of formate remained at 80% for 50 h at high partial current densities (>100 mA cm −2 ). In-situ Raman spectra and density functional theory calculations confirmed that copper doping lowers the energy barrier of HCOO − formation on the Bi (012) plane and increases the conductivity of the carbon nanofiber network. Due to the well-designed conductive framework and the highly dispersed BiCu active sites, this hybrid membrane shows high activity, high selectivity, and long stability simultaneously.
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Science Advances
·
2023
·Vol. 9
·期 24
·
IF 13.6
Mingrui Wang,Peng Wang,Guanghui Zhang,Zening Cheng,Mengmeng Zhang,Yulong Liu,Rongtan Li,Jie Zhu,Jianyang Wang,Kai Bian,Yi Liu,Fanshu Ding,Thomas P. Senftle,Xiaowa Nie,Qiang Fu,Chunshan Song,Xinwen Guo
The decomposition of cobalt carbide (Co 2 C) to metallic cobalt in CO 2 hydrogenation results in a notable drop in the selectivity of valued C 2+ products, and the stabilization of Co 2 C remains a grand challenge. Here, we report an in situ synthesized K-Co 2 C catalyst, and the selectivity of C 2+ hydrocarbons in CO 2 hydrogenation achieves 67.3% at 300°C, 3.0 MPa. Experimental and theoretical results elucidate that CoO transforms to Co 2 C in the reaction, while the stabilization of Co 2 C is dependent on the reaction atmosphere and the K promoter. During the carburization, the K promoter and H 2 O jointly assist in the formation of surface C * species via the carboxylate intermediate, while the adsorption of C * on CoO is enhanced by the K promoter. The lifetime of the K-Co 2 C is further prolonged from 35 hours to over 200 hours by co-feeding H 2 O. This work provides a fundamental understanding toward the role of H 2 O in Co 2 C chemistry, as well as the potential of extending its application in other reactions.
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Frontiers of Chemical Science and Engineering
·
2025
·Vol. 19
·期 12
·1-12
·
IF 4.5
Song Jinbo,Jing Jieying,Zhang Jinpeng,Xu Yufeng,Li Wen-Ying
Alkaline metal salt-promoted MgO sorbents are effective for CO 2 capture, but they face challenges with decreased CO 2 capture performance and powder elutriation in practical applications, arising due to the loss of pore structures and poor mechanical strength of alkaline metal salt-promoted MgO sorbent powder. Herein, granulation technology was employed to resolve the above problem. The optimized alkaline metal salt-promoted MgO sorbent pellets exhibited a CO 2 capture capacity of 11.46 mmol·g −1 and a mechanical strength of 11.14 MPa. This mechanical strength was nearly three times greater than that of alkaline metal salt-promoted MgO sorbent pellets without granulation promoters. After 20 cycles, CO 2 capture capacity stabilized at 8.71 mmol·g −1 , while mechanical strength was maintained at 8.92 MPa. Through characterization, it was revealed that the pore structure generated by the pyrolysis of the granulation promoters notably increased the specific surface area, leading to high CO 2 capture capacity. Meanwhile, the strengthened mechanical strength of the alkaline metal salt-promoted MgO sorbent pellets was primarily due to the in situ formation of a γ -AlOOH sol-gel cluster skeleton. Thus, this study provides an effective technological pathway to enhance the performance of the alkaline metal salt-promoted MgO sorbent pellets for industrial applications.
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Yadan Yu,Wenyu Li,Huiting Qiao,Yuyu Liu,Momo Safari,Haitao Huang,Jinli Qiao
CO 2 electroreduction enables the sustainable conversion of greenhouse gases into value-added chemicals, thereby reducing global warming. In this study, a bismuth–samarium (Bi–Sm) bimetallic catalyst (Bi 4 Sm 1 ) was prepared, exhibiting excellent performance for the CO₂-to-formate electrosynthesis facilitated by situ-generated nanosheets. The incorporation of Sm into Bi catalyst enriched the active sites on the catalyst surface, achieving excellent stability (>150 h) and high formate selectivity (Faradaic efficiency, FE formate = 93.74%) with a current density of 13.5 mA cm -2 at −1.0 V vs. reversible hydrogen electrode (V RHE ) in a H-cell reactor containing 0.5 M KHCO 3 electrolyte. Moreover, in a flow cell containing 1M KOH electrolyte, the catalyst achieved a current density exceeding 162 mA cm -2 at -0.7 V RHE , with a slight decrease in FE formate (92.55%). This catalyst outperformed most reported catalysts, highlighting its large-scale potential applications.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Xianda Zhang,Yaotian Yan,Yangshuo Liu,Chun Li,Jian Cao,Junlei Qi
CO2 reduction reaction (CO2RR) has been considered as a promising process that can compensate CO2 emission and convert it into value-added chemicals. In preparation of CO2RR catalytic electrode, Nafion is a common binder but its effect in catalytic process is usually ignored. Herein, we proposed the bifunction of Nafion in CO2RR based on its molecular structure and successfully developed a CO2-affinitive surface of Micro-Ag /Nafion by controlling the content of Nafion, which exhibited a superior CO faradaic efficiency (FECO) of 95.07% at -0.9 V (vs. RHE). This excellent FECO and 2 times of CO partial current density (jCO) in flow-cell proved its industrial prospect. Its splendid selectivity of CO2RR was attributed to the selective polarization of CO2 molecule at Nafion, which resulted in the 6.8 times higher adsorption energy (Eads) of CO2 than H2O. Therefore, CO2RR gained an advantage in the competitive reaction.Nafion was recognized as a favorable transporter for CO2 on the surface of metal catalyst. Our work describes the bifunctional role of Nafion in CO2RR electrode and it will contribute to optimize the design of metal/Nafion catalytic material for CO2RR.
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MOLECULES
·
2025
·Vol. 30
·期 12
·2626
·
IF 4.6
Minhui Pan,Linlin Zheng,Congyu Cai,Weiwei Wang
The photocatalytic reduction of CO2into valuable hydrocarbons presents significant potential. In this research, a ZnO/ZnAl2O4composite photocatalyst was synthesized using the hydrothermal method, resulting in a marked enhancement in CO yield—approximately three times greater than that achieved with pure ZnAl2O4nanoparticles. The formation of a Z-scheme heterojunction between ZnO and ZnAl2O4was observed, characterized by low interfacial charge transfer resistance, an abundance of reaction sites, and optimized charge transport pathways. Within this composite, ZnO contributes additional vacancies, thereby increasing active sites and enhancing the separation and migration of photogenerated carriers. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analysis indicates that ZnAl2O4facilitates the formation of key intermediates, such as *COOH and HCO3−, thus promoting the conversion of CO2to CO. This study offers valuable insights into the design of heterogeneous catalysts with diverse active components to enhance the performance of CO2photocatalytic reduction through synergistic effects.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Hang Zhou,Xiaomeng You,Zejiang Huang,Beibei Xu,Yingli Shi,Xuelu Wang,Ye-Feng Yao
Dual-atom catalysts, which combine the strengths of single-atom catalysts and metal alloys, are considered optimal for facilitating electrocatalytic CO 2 reduction processes. However, developing the means of enhancing the utilization efficiency of bimetallic atoms at catalytic sites and controlling the complex atomic coordination environment to achieve high selectivity and Faradaic efficiency remain a challenge. The present work addresses this issue by synthesizing a bimetallic SnCu-WC x catalyst via the introduction of individual Sn and Cu atoms supported on a tungsten carbide substrate. High Faradaic efficiencies of 98.62 % and 90.19 % at current densities of 100 and 500 mA cm −2 for the reduction of CO 2 to formate are respectively achieved through modulation of the coordination environment and electron/proton transfer during catalysis, the creation of shared adsorption sites, and the promotion of synergistic electrocatalysis. The results of operando nuclear magnetic resonance spectroscopy indicate that activated *OH groups are involved in the formation of formate due to the affinity of individual Sn atoms in the SnCu-WC x catalyst toward *OH. Density functional theory calculations confirm that the presence of individual Sn atoms in SnCu-WC x promotes the dissociation of H 2 O, and thereby modulates the catalytic microenvironment to accelerate the kinetics for the conversion of activated *CO to *COOH groups. Accordingly, the proposed strategy offers new insights into the design of bimetallic catalysts.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Si-Mian Liu,Qian Liang,Mu-Lan Yao,Xiao Wang,Long Tang,Er-Lin Yue,Ji-Jiang Wang,Xiang-Yang Hou
The excessive existence of CO 2 in the atmosphere has caused serious environmental problems. Therefore, how to capture, selectively adsorb, and the effective utilization of CO 2 into useful chemicals has attracted widespread attention. In particular, the exploration of combining CO 2 capture with conversion has rarely been reported. Herein, two isometric metal-organic frameworks (MOFs) Cd 3 (ntba) 2 -(2,2′-bipy) 2 ] n (MOF1), and Co 3 (ntba) 2 (2,2′-bipy) 2 ] n (MOF2) were successfully obtained. Under normal temperature and pressure conditions, based on the ideal specific surface area porosity, MOF1 and MOF2 exhibit super adsorption and separation ability for CO 2 . The maximum adsorption capacity and separation ratio are 54.3 cm 3 g -1 (MOF1), 64.2 cm 3 g -1 (MOF2), and 16.9 (MOF1, CO 2 /CH 4 ), 192.7 (MOF1, CO 2 /N 2 ), 117.8 (MOF1, CO 2 /O 2 ), 22.6 (MOF2, CO 2 /CH 4 ), 130.3 (MOF2, CO 2 /N 2 ), 59.1 (MOF2, CO 2 /O 2 ), respectively. Under optimal reaction conditions, the MOF1 and MOF2 as catalysts demonstrate outstanding efficiency and reaction selectivity in catalyzing cycloaddition conversion reaction of CO 2 , achieving yields of 96% and 93%, respectively. The catalytic reaction produced useful chemical products via a novel method integrating CO 2 capture and conversion, eliminating the economic costs associated with CO₂ purification and enabling the economical utilization of CO₂ . Thus, this work presents a novel strategy for the CO 2 utilization in mixed gases and can also provide valuable references for related research.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shuangshuo Li,Yongjing Hao,Xionglei Wang,Zheng Zhu,Fan Li,Jiaojiao Zhao,Tian Tian,Tao Chang
In addressing the critical challenge of achieving functional synergy in sustainable materials, this study introduces an innovative ionic-pair strategy to construct amino acid-derived green organic polymer frameworks with specifically tailored active sites for CO 2 adsorption and conversion, devoid of halide anions and metal ions. The intrinsic properties and microstructure of these polymers were meticulously modulated through ionic-pairing between amino acid monomers. Comprehensive characterizations and molecular dynamic simulations systematically verified the presence of dual-active sites and stability of the architecture. Experimental and kinetic analyses indicate that these polymers exhibit exceptional performance in CO 2 adsorption capacity and catalytic conversion, with an activated energy of 15.76 kcal·mol −1 . Furthermore, the adsorption and catalytic mechanisms were extensively investigated using the Monte Carlo method and density functional theory calculations. The amino group in AMA-Glu effectively adsorbs and activates CO 2 , while epoxides undergo nucleophilic attack by the carboxylate anion, facilitating ring-opening reactions. The synergistic interaction between the two groups promotes the cycloaddition reaction. Under conditions devoid of co-catalyst, solvent, and halogen at 80 °C for 8 h, the yield of cyclic carbonates achieved 94.3 %, demonstrating strong competitive performance. This study offers substantial theoretical and practical insights into the utilization of green organic catalytic materials for CO 2 conversion.
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Processes
·
2025
·Vol. 13
·期 9
·2903
·
IF 2.8
Ping Guo,Yong Li,Yanbao Liu,Yunlong Zou
In this study, a new type of double crosslinked nanospheres (DCNPM-A) was developed to solve the problem of gas channeling caused by fracture development in the process of CO2oil displacement, and the microsphere system with delayed swelling was successfully synthesized by inverse micro lotion polymerization. The microsphere adopts a dual crosslinking structure of stable crosslinking agent (MBA) and unstable crosslinking agent (UCA), achieving intelligent sealing function of shallow low expansion and deep high temperature triggered secondary expansion. The successful preparation of microspheres was verified by characterization methods such as Zeta potential and SEM, and the effects of reaction temperature, time, initiator and crosslinking agent dosage on microsphere properties were systematically studied. The experimental results show that DCNPM-A microspheres exhibit excellent expansion performance, thermal stability, and acid resistance in acidic, high-temperature, and high mineralization environments. Their expansion ratio can reach 13.5 times, and they can maintain stability for more than 60 days in supercritical CO2environments. Core displacement experiments have confirmed that the microspheres have the best sealing performance in matrices with a permeability of 10 × 10−3μm2and fractures with a width of 0.03 mm. The combination of 0.8 PV injection volume, 0.5 mL·min−1injection rate, and continuous injection method significantly improved the plugging rate and recovery rate of CO2flooding. This study provides new technical support for the efficient development of low-permeability fractured reservoirs.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shang-Yuan Cheng,Chen-Peng Zhang,Meng-na Chao,Shu-Wei Guo,Gui-Sheng Qi
Suspended nanodroplets affect the transfer process within fluids through micro-perturbation or micro-convection effects. Therefore, adding dispersed nanodroplets as the dispersed phase into the liquid phase to form nanoemulsions can enhance the CO 2 absorption process. The quality of nanoemulsions mainly depends on the emulsification equipment. Traditional physical mechanical effects can only achieve large-scale macroscopic mixing, which usually takes a long time to complete, resulting in issues such as low production efficiency, batch operation, and long preparation cycles. This paper uses an impinging stream-rotating packed bed as a reactor, with span60 and tween60 as surfactants, and adopts a high-gravity process intensification technology to prepare undecane/methanol nanoemulsions with good dispersion stability. Nanoemulsion absorbents for CO 2 capture applications have been developed. The effects of different operating conditions on the dispersion stability of nanoemulsion were investigated. Furthermore, CO 2 absorption performance of nanoemulsion absorbents and methanol were investigated in a bubbling reactor. Based on the results, the reasonable mechanism for the enhancement of mass transfer was also discussed in detail. Further experiments on CO 2 absorption using nanofluids were conducted and compared with pure methanol. The results indicate that when the undecane volume fraction is 0.01 %, the high-gravity factor is 27, the impinging velocity is 14.1 m·s −1 , and the circulation time is 20 min, the nanoemulsion exhibits the highest stability, with the narrowest particle size distribution of oil droplets, an average particle size of 20.5 nm, and the highest uniformity. Simultaneously, the change in turbidity over time is minimal. The corresponding thermal conductivity at 25°C is 0.2003 W/m·K. The addition of nano-oil droplets significantly accelerates the CO 2 absorption rate, allowing the absorbent to reach saturation earlier, while the total amount of CO 2 absorbed remains the same. Compared with pure methanol, the nanoemulsion enhances the CO 2 absorption rate by 4.48 %. This work may provide a promising green method for efficient production of nanoemulsions for carbon dioxide capture.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Dun Zhou,Hongbo Zhang,Yulong Rao,Xiaobai Li,Huihui Zhang,Yongpeng Liu,Hongwei Ma
CO 2 capture and release are critical for enhancing photosynthetic efficiency of plants and biomass accumulation. However, achieving efficient capture and directional transport of CO 2 to plants near the source of carbon emissions to boost photosynthetic efficiency are mains an important technical challenge. In this study, we introduce an innovative strategy for fabricating a cellulose-based CO 2 -capture foam-like porous material-DGP, which can significantly enhance the photosynthetic efficiency of tobacco plants. By chemically crosslinking superbranched amino polymers on a lignocellulose substrate, DGP not only exhibits excellent CO 2 capture capacity of 8.01 mmol g −1 at room temperature, but also achieves an effective slow release of CO 2 with a release rate of up to 51 % and a duration of up to 10 h without additional energy input. This characteristic allows DGP to simulate the CO 2 concentration mechanism of plants in nature, thereby increasing the net photosynthetic efficiency of tobacco by 70 % and the intercellular CO 2 concentration by 52 %, which significantly promotes the accumulation of biomass. The utilization of this material has broad application prospects for enhancing the carbon sink capacity of the ecosystem, mitigating the greenhouse effect and improving crop yield.
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