Journal of CO2 Utilization
·
2021
·
IF 7.132
Danqing Shu,Miao Wang,Fengyu Tian,Honglei Zhang,Chuang Peng
Electroreduction of CO 2 to high value-added products such as hydrocarbons provides a promising way to create a carbon neutral circular economy. Copper (Cu) is the most effective metal catalyst with selectivity towards hydrocarbons but Cu catalyst alone generally produces hydrocarbons at low selectivity and yield. Operando surface enhanced infrared absorption spectroscopic (SEIRAS) analysis reveals that the low hydrocarbon yield is attributed to the poor ability of Cu to produce carbon monoxide (CO), which is a crucial intermediate for hydrocarbon formation. In the current study, an Ag-Cu dual-cathode CO 2 RR device is developed, which allows separate control of electrode potential. This dual-cathode cell shows increased hydrocarbon yield (83 % for methane and 106 % for ethylene) and a 200 mV lower onset potential for C 2 H 4 , compared to electrolysis with a single Cu cathode. The CO produced by the Ag cathode transfers to Cu and increase its CO coverage, facilitating methane formation as well as promoting C C coupling to form ethylene. This study also reveals a mismatch of optimum electrode potential between Ag and Cu, which results in compromised performance of the two components in an Ag-Cu bimetallic electrocatalyst, but poses no challenge in the dual-cathode cell. To optimize the performance of the dual-cathode cell, we propose the use of a single-pass dual-gas-diffusion-cathode reactor with enhanced mass transfer for maximum hydrocarbon production. This work verifies that splitting the complex CO 2 RR process into two separate steps is a feasible method to improve the overall efficiency and rate of advanced products while reducing the energy input.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jingyun Qian,Wenna Zhang,Xue Yang,Kexin Yan,Meikun Shen,Hongyue Pan,Hongjun Zhu,Lei Wang
Constructing the metal cation-mediated low-cost inorganic sorbent with high separation efficiency in CO 2 , N 2 , and CH 4 remains a major challenge. Herein, we developed a series of alkali metal cations (Na + , K + , Rb + , Cs + )-exchanged ERI zeolites and adopted in the separation process of CO 2 among the gas mixture. Among the ion-exchanged zeolites, the zeolite K-ERI showed a high adsorption volume of 70.84 cm 3 g −1 and an IAST selectivity of CO 2 /CH 4 : 6254, CO 2 /N 2 : 2872 at 298 K, respectively, far outweighed the reported metal cation exchanged zeolites. Combining powder X-ray diffraction crystallography and density functional theory calculations, we unequivocally unveiled that the metal cations located at s 8 r effectively tailored zeolite aperture, and metal cation-gas molecules interactions synergically restrained the pass-through capacity of CO 2 in ion-exchanged ERI framework. Such a unique host–guest interaction governed by metal cations in aluminosilicate zeolite ERI affords a general strategy for gas separation.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2016
·
IF 2.196
Yong-Jie Geng,Jie Wang,Zhi-Hong Liu
Two transition metal borates with microporous structures for Na 2 Co 2 B 12 O 21 and Na 2 Cu 2 B 12 O 21 have been synthesized and characterized by XRD, FT-IR, and elemental analysis. The molar enthalpies of solution of Na 2 Co 2 B 12 O 21 (s) and Na 2 Cu 2 B 12 O 21 (s) in 1 mol dm −3 HCl(aq) were measured by microcalorimeter at T = 298.15 K, respectively. The molar enthalpies of solution of CoCl 2 ·6H 2 O(s) and CuCl 2 ·2H 2 O(s) in the mixture solvent of 2.00 cm 3 of 1 mol dm −3 HCl(aq) in which 5.30 mg of H 3 BO 3 and 0.84 mg of NaCl being added were also measured, respectively. With the incorporation of the previously determined enthalpy of solution of H 3 BO 3 (s) in 1 mol dm −3 HCl(aq), together with the standard molar enthalpies of formation for CoCl 2 ·6H 2 O(s)/CuCl 2 ·2H 2 O(s), NaCl(s), H 3 BO 3 (s), HCl(aq) and H 2 O(l), the standard molar enthalpies of formation of – (9072.4 ± 9.7) kJ mol −1 for Na 2 Co 2 B 12 O 21 (s) and – (8887.5 ± 9.7) kJ mol −1 for Na 2 Cu 2 B 12 O 21 (s) at T = 298.15 K were obtained on the basis of the appropriate thermochemical cycles. It is obvious that Na 2 Co 2 B 12 O 21 (s) is more thermal stable than that of Na 2 Cu 2 B 12 O 21 (s).
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高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2021
·Vol. 2021
·期 35
·3601-3610
·
IF 2.524
Shaozhong Li,Qing Guo,Jin Li,Yongke Hu,Jiayu Lin
Graphical The mesostructured Cu/AlZnO-9 catalyst with 15 wt % Cu was prepared for the hydrogenation of CO 2 to methanol. The well mesostructure increased the exposed Cu surface area and CO 2 adsorption sites, which accelerated the CO 2 conversion, and the ZnO in catalyst increased the generation of methanol. In addition, the well mesostructure heightened the stability of supported Cu catalyst due to the high dispersion of Cu nanoparticles. In this work, the mesostructured Cu/AlZnO catalysts were prepared for the CO 2 hydrogenation to methanol. Experimental results showed that the weight ratio of Al 2 O 3 and ZnO affected the morphology of the mesoporous AlZnO supports and surface properties of the mesostructured Cu/AlZnO catalysts. The AlZnO-9 (the Al 2 O 3 mass within the AlZnO support was 90 wt%) with loose spongy porous structure and high surface area facilitated the Cu nanoparticle dispersion. Thus, the Cu/AlZnO-9 catalyst showed higher exposed Cu surface area ( S Cu ) and more exposed CO 2 adsorption sites, which accelerated the CO 2 conversion. Meanwhile, the ZnO added into catalysts increased the strength of surface basicity and the surface concentration of Zn species, which promoted the catalytic activity of CO 2 hydrogenation to methanol. In addition, the well mesostructure heightened the stability of supported Cu catalyst due to the high dispersion of Cu nanoparticles.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Changqing Gui,Zirui Wang,Changjian Ling,Zhongfeng Tang
Molten salt-doped MgO adsorbent is considered one of the most promising CO 2 adsorbents in the field. In this work, MgO-based adsorbents were prepared by one-step calcination using MgCl 2 ·6 H 2 O as magnesium source. The CO 2 adsorption performance of MgO-based adsorbents was investigated via different methods. Results showed that the maximum CO 2 adsorption capacity of MgO doped by LiNO 3 -NaNO 3 -KNO 3 was 57.1% at the CO 2 concentration of 80% and 350 ℃, and the MgO-based adsorbents showed good regeneration. The nanosheet structure of the MgO-based adsorbents decreased with the increase in the number of cycles, whereas the crystal structures of MgO and alkali metal nitrates did not change because of multiple decarbonization. DFT computation revealed selective adsorption of CO 2 on different crystal faces of MgO. The (200) crystal face of molten salt-doped MgO did not have CO 2 trap ability. In addition, the doped nitrate did not directly participate in the reaction but reduced the adsorption energy of MgO carbonation. The adsorption energies of the MgO (220) and (222) crystal faces after doping with nitrate were reduced to − 2.07 and − 3.26 eV, respectively. The overall energy level of adsorption decreased as the number of resonance peaks and the stability of the structure increased. This study explains why MgO currently fails to reach the theoretical adsorption capacity and reveals the underlying mechanism of molten salts.
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高影响因子
Advanced Fiber Materials
·
2019
·Vol. 1
·期 3
·222-230
·
IF 0
Liang Liping,Dong Yanyan,Wang Hongfang,Meng Xu
Stimuli-responsive materials with switchable wettability have promising practical applications in oil/water separation. A novel CO 2 -responsive cotton fabric for controlled oil/water separation was fabricated based on mussel-inspired reaction and polymerized with 2-(dimethylamino)ethyl methacrylate (DMAEMA). As expected, the modified fabric exhibited switchable hydrophilicity and hydrophobicity after CO 2 /N 2 alternation, and it could be used for gravity-driven CO 2 -controlled oil/water separation. Water was selectively penetrated through the fabric and separated from oil after treating by CO 2 . A reversed wettability could be generated through simply treated with N 2 . It is expected that the as-prepared fabrics could be applied in smart oil/water separation due to the attractive properties of CO 2 -switchable system.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
·
IF 3.764
Wenjian Yue,Zhiyu Huang,Mengli Xiao,Xiaojiang Li,Wenjing Ma,Ying Zhang,Shanshan Dai,Hongsheng Lu
In this article, a higher fatty acid-based ternary CO2-controllable dual-circulation had been successfully constructed, where it provided an excellent oil recovery performance and all solvents could be cycled. This dual-circulation adopted the oil-soluble higher fatty acid (HFA) as the outside loop to extract oil and selected poly(propylene glycol) bis(2-aminopropylether) (Jeffamine D230) as the inner loop to impel the outside loop. In washing oil technology, D230 and HFA as cleaning solvents are ideal substitutes for traditional tertiary amines. First, there is the electrostatic interaction between HFA (represented by n-decanoic acid) and D230, as detected by 1H MNR. The circulation of the system is supported by the rapid CO2-switchable behaviors of HFA-D230, where the reversible phenomenon was recorded by a pH meter and a conductivity meter. In addition, the HFA/D230/water system has demonstrated the cyclic process of dissolving the oil in the simulated oil (the dodecane, kerosene, and diesel) recovery experiment. Finally, the n-decanoic acid (C10-HFA)/D230/water ternary dual-circulation system was obtained as the optimal scheme due to its excellent recovery and separation property. During the separation of simulated oil by using the C10-HFA/D230/water system, the recovery rate of the simulated oil was more than 93% and there was no residual n-decanoic acid by GC/MS analysis. This dual-circulation was successfully established, providing a new method to replace the traditional tertiary amine for oil recovery.
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高影响因子
RSC Advances
·
2018
·Vol. 8
·期 19
·10347-10354
·
IF 2.936
Shuangshuang Hou,Shaolei Wang,Xuejun Long,Bien Tan
In order to achieve efficient CO2 capture, four novel microporous organic polymers, based on distinct polycyclic aromatic hydrocarbons such as fluoranthene, binaphthalene, naphthalene and phenanthrene, were successfully prepared by the solvent knitting method. N2 sorption isotherms indicate that these polymers are predominately microporous with ultrahigh BET surface area i.e., 1788 m2 g−1 for fluoranthene-based Polymer 1, 1702 m2 g−1 for binaphthalene-based Polymer 2 and objective CO2 uptake capacity of 24.79 wt% and 20.19 wt% (273.15 K/1.00 bar) respectively. While compared with the former two polymers, though 1227 m2 g−1 and 978 m2 g−1 are moderate in surface area, however the naphthalene-based Polymer 3 and phenanthrene-based Polymer 4 still exhibit CO2 adsorption of up to 17.44 wt% and 18.15 wt% respectively under the similar conditions. Moreover, the H2 storage and CH4 adsorption in these polymers can be 2.20 wt% (77.3 K/1.13 bar) and 2.79 wt% (273.15 K/1.00 bar). More significantly, the electron-rich PAHs are proved to be new building blocks that provide a wealth of chances to produce hypercrosslinked polymers with efficient gas adsorption capacity, which are greatly influenced by the porous nature of polymers. Given the merits including mild reaction conditions, low cost, high surface area, impressive gas absorption performance, high thermal stability, these polymers are considered to be promising candidates for CO2 capture and energy storage under more practical conditions.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Yanpeng Chen,Xing Zhu,Kongzhai Li,Yonggang Wei,Yane Zheng,Hua Wang
Syngas generation via thermochemical H2O–CO2 splitting relies heavily on a high-temperature decomposition of metal oxides into a reduced state. Meanwhile, typical chemical looping partial oxidation of methane to syngas suffers from the carbon deposition and the low selectivity toward syngas. To overcome these drawbacks, the partial oxidation of methane and H2O–CO2 splitting are coupled to consist of an alternative chemical looping redox scheme for the generation of Fischer–Tropsch (F–T)-ready syngas. The usability of lattice oxygen in a redox catalyst is facilitated, and its redox property is also thermodynamically optimized by using H2O and CO2 as soft oxidants, guaranteeing an effective generation of syngas from both redox steps. The carbon tolerance is greatly enhanced due to H2O or CO2 gasification in the reoxidization step. Experimental studies confirm the redox scheme by using CeO2–LaFeO3 redox catalyst, demonstrating generation of syngas with an H2/CO molar ratio around 2.0 in both methane partial oxidation and H2O–CO2 splitting steps over 30 repeated cycles at 850 °C. A syngas selectivity of 95% in methane partial oxidation and nearly 100% conversion of CO2 to CO can be achieved. Synergistic effect and competing reaction between H2O and CO2 splittings over the reduced redox catalyst are the key factors for the control of syngas composition and the intensification of CO2 splitting. The proposed approach can potentially be applied for production of F–T-ready syngas with an increased yield without the need for gas separation when compared to the state-of-the-art thermochemical splitting or methane chemical looping partial oxidation processes.
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高影响因子
Science China-Chemistry
·
2020
·Vol. 63
·期 12
·1727-1733
·
IF 6.356
Ren Xinyi,Liu Song,Li Huicong,Ding Jie,Liu Linghui,Kuang Zhichong,Li Ling,Yang Hongbin,Bai Fuquan,Huang Yanqiang,Zhang Tao,Liu Bin
Electrochemical carbon dioxide reduction reaction (CO 2 RR) powered by renewable electricity offers an attractive approach to reduce carbon emission and at the same time produce valuable chemicals/fuels. To design efficient CO 2 reduction electrocatalyst, it is important to understand the structure-activity relationship. Herein, we design a series of single Co atoms electrocatalysts with well-defined active sites electronic structures, which exhibit outstanding CO 2 RR activity with controllable selectivity to CO. Experimental and density functional theory (DFT) calculation studies show that introducing nitro (amino) ligand next to single Co atom catalytic center with electron-withdrawing (electron-donating) capability favors (hinders) CO 2 reduction catalysis. This work provides an in-depth understanding of how functional ligand affects the splitting of transition metal 3d electron orbital, thereby changing the electron transfer from transition metal active site to CO 2 , which is closely related to the Gibbs free energy of the rate-determining step (CO 2 +e − +*→*CO 2 − ).
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高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Hao Li,Zhuo Chen,Rongxin Xia,Ze Zhang,Junhu Zhou,Yu-You Li,Jun Cheng
To simultaneously promote both direct (via electron carriers) and indirect electron transfer (via hydrogen carriers) in the microbial electroreduction of CO2 to CH4, FeCoCrNiMo high-entropy alloys (HEAs) combined with methanogens were proposed herein. Experimental results showed that spherical HEA heterostructures significantly enhanced the electrical conductivity and catalytic activity. FeCoCrNiMo HEAs increased the abundance of hydrogenotrophic methanogens (e.g., Methanobacterium) and electroactive bacteria (e.g., Ureibacillus), as well as the expression of conductive pilus-associated gene (pilA) to promote electron transfer. FeCoCrNiMo HEAs also increased the content of aromatic proteins and tryptophan in extracellular polymeric substances, enhancing biofilm conductivity, while the uniform dispersion of the five metal elements reduced both biofilm resistance and charge transfer resistance. Therefore, HEAs enhanced the maximum methane production rate by 6.58 times (2.17 mmol L–1 day–1) with 90.6% faradaic efficiency. This study demonstrated that FeCoCrNiMo HEAs promoted electron shuttling efficiency, biofilm electroactivity, and stability, highlighting their potential as multifunctional promoters for driving CO2 reduction to methane.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shuyi Xia,Xiang Wang,Deqi Fan,Yingying Li,Yi Lu
Freshwater scarcity and rising atmospheric CO 2 are two pressing environmental challenges. Here we report a multifunctional electrospun bilayer nanofibrous membrane that integrates solar-driven interfacial water evaporation with photocatalytic CO 2 reduction in a single platform. The top PAN/CNT layer delivers broadband solar absorption and efficient photothermal conversion, while the bottom CoAl-LDH/PAN layer provides catalytic sites and capillary-assisted water transport, stabilizing a three-phase reaction interface. Under one-sun illumination, the bilayer nanofibrous membrane achieves a water evaporation rate of 2.5 kg·m −2 ·h −1 and the CAL/PAN-6 % layer within it delivers a CO evolution rate of 287.6 μmol·g −1 , both outperforming single-layer counterparts. Spectroscopic and electrochemical analyses reveal suppressed charge recombination and enhanced carrier lifetimes, and outdoor tests confirm robust operation under fluctuating sunlight. The solvent-based but recyclable electrospun architecture presents a scalable environmental materials platform that couples clean water supply with carbon mitigation, offering a viable route toward sustainable water-energy-carbon integration.
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高影响因子
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