ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Weida Chen,Meisi Chen,Tong Lei,Feng Zhang,Jiao Geng
High regeneration energy is a critical barrier to the large-scale implementation of CO2 capture technologies. To address this challenge, we present a novel energy-efficient biphasic absorbent system, designed by incorporating sterically hindered amine ionic liquids (AMP-TZ) with N,N,N′,N′-tetramethyl-1,6-hexanediamine (TMHDA). The innovative design focuses on enhancing the spatial site resistivity of ionic liquids, which plays a key role in optimizing the CO2 absorption and minimizing regeneration energy. This system demonstrates superior performance, achieving a CO2 absorption capacity of 2.72 mol/kg at 313.2 K and 150 kPa, with a low regeneration energy of 2.31 GJ/t of CO2. Molecular dynamics simulations and quantum chemical calculations reveal that AMP-TZ promotes proton transfer during absorption and stabilizes bicarbonate (HCO3–) in the CO2-rich phase via weak hydrogen bonding. The unique role of AMP-TZ as a bifunctional hydrogen bond donor/acceptor and its ability to suppress the self-aggregation of HCO3– enhance both the absorption efficiency and regeneration performance. This study provides insights into the design of low-hydration CO2 capture systems and offers a theoretical framework for developing highly efficient, energy-saving biphasic absorbents.
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INORGANIC CHEMISTRY
·
2024
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IF 4.3
Hongyu Ma,Xi Wu,Xinghua Li,Jie Liu,Haipeng Dong,Yu Liu,Luyao Niu,Fang Zhang,Wenbo Wang,Changlu Shao,Xiaowei Li,Yichun Liu
Photocatalytic carbon dioxide (CO2) reduction for high-value hydrocarbon fuel production is a promising strategy to tackle global energy demand and climate change. However, this technology faces formidable challenges, primarily stemming from low yield and poor selectivity of C2 products of the desired hydrocarbon fuels. This study reported ZnO/ZnCo2O4 Janus hollow nanofibers (ZnO/ZCO JHNFs) prepared by electrospinning and atomic layer deposition. Photocatalytic tests revealed an ethanol yield of 4.99 μmol g–1 h–1 for ZnO/ZnCo2O4 JHNFs, surpassing mixed ZnO/ZnCo2O4 nanofibers (ZnO/ZCO NFs) by 4.35 times and pure ZnO by 12.7 times. The selectivity of 58.8% is 2.38 and 4.49 times higher than those of ZnO/ZnCo2O4 NFs and ZnO, respectively. These enhancements are attributed to efficient carrier separation facilitated by the ordered internal electric field of the Z-scheme heterojunction interface, validated by the energy band evaluations from experimentation and density functional theory (DFT) simulations and charge separation characterizations of photocurrent, impedance, and photoluminescence spectra. The Janus structure also effectively exposes the surface of ZnCo2O4 to CO2 molecules, increasing the active site availability, as confirmed by BET nitrogen adsorption/desorption, temperature-programmed desorption tests, and DFT adsorption energy calculations. This study proposes a novel approach for efficient photocatalytic hydrocarbon fuel production, with potential applications in energy and climate crisis mitigation.
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Small
·
2024
·Vol. 20
·期 31
·2310894
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IF 13
Jie Chen,Yang Liu,Quanhua Xie,Yuanyuan He,Dengjie Zhong,Haixing Chang,Shih-Hsin Ho,Nianbing Zhong
A visible-light-driven CO 2 reduction optical fiber is fabricated using graphene-like nitrogen-doped composites and hollow quartz optical fibers to achieve enhanced activity, selectivity, and light utilization for CO 2 photoreduction. The composites are synthesized from a lead-based metal–organic framework (TMOF-10-NH 2 ) and g-C 3 N 4 nanosheet (CNNS) via electrostatic self-assembly. The TMOF-10-NH 2 /g-C 3 N 4 (TMOF/CNNS) photocatalyst with an S-type heterojunction is coated on optical fiber. The TMOF/CNNS coating, which has a bandgap energy of 2.15 eV, has good photoinduced capability at the coating interfaces, high photogenerated electron–hole pair yield, and high charge transfer rate. The conduction band potential of the TMOF/CNNS coating is more negative than that for CO 2 reduction. Moreover, TMOF facilitates the CO desorption on its surface, thereby improving the selectivity for CO production. High CO 2 photoreduction and selectivity for CO production is demonstrated by the TMOF/CNNS-coated optical fiber with the cladding/core diameter of 2000/1000 µm, 10 wt% TMOF in CNNS, coating thickness of 25 µm, initial CO 2 concentration of 90 vol%, and relative humidity of 88% RH under the excitation wavelength of 380–780 nm. Overall, the photocatalytic hollow optical fiber developed herein provides an effective and efficient approach for the enhancement of light utilization efficiency of photocatalysts and selective CO 2 reduction.
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ChemistrySelect
·
2024
·Vol. 9
·期 44
·e202403927
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IF 1.9
Hui Han,He Cui,Jiabo Wang,Kai Ge,Yongfang Yang
Graphical In this paper, 2D MOF-Co, 2D MOF-Co/Cu, and 2D MOF-Co/Cu/Fe are designed and prepared using 1,4-benzendicarboxylic acid (1,4-BDC) as organic ligands. Their charge transfer, separation efficiency, and effects on photocatalytic CO 2 reduction are studied. The results show that 2D multimetallic MOF-Co/Cu/Fe has better photocatalytic CO 2 reduction activity, so it has higher research value and development prospect in the field of photocatalytic CO 2 reduction. In this study, 2D multimetallic MOFs combined with the advantages of 2D nanosheets, with the synergetic effect of multimetallic nodes, exhibited good photocatalytic activity for reduction of CO 2 . Herein, a 2D MOF-Co/Cu/Fe were successfully prepared via one-pot stirring of the solutions of multimetal salts and organic ligands at room temperature. Introduction of the second and third metal (Cu and Fe) into MOF-Co does not change the 2D morphology of MOFs, although it improved the photocatalytic CO 2 reduction performance by broadening the light absorption range of 2D MOF-Co, accelerating the separation efficiency and transfer rate of photogenerated carriers. Upon irradiation with full-spectrum light, the average CO yield of 2D MOF-Co/Cu/Fe achieved 17.06 µmol·g −1 ·h −1 , being about 1.8 and 1.2 times that of 2D MOF-Co and 2D MOF-Co/Cu. This work provides an insight into 2D multimetallic MOFs-based photocatalysts in catalytic CO 2 reduction.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Yunchuan Pu,Guangwei He,Mingang Zhao,Ziqi Yang,He Li,Yanxiong Ren,Mengying Long,Xuerui Wang,Dan Zhao,Zhongyi Jiang
Two-dimensional metal-organic frameworks (2DMOFs) have emerged as highly appealing candidates as advanced separation membrane materials. However, constructing 2DMOF membranes with appropriate channel sizes to separate CO 2 from N 2 remains a great challenge. Here, we propose an in-situ crystallization approach to synthesize CO 2 -philic-polymer functionalized Zr-based MOF nanosheets, enabling the fabrication of efficient CO 2 capture membranes. The in-situ MOF crystallization with polyethylenimine (PEI) polymers leads to a uniform distribution of amines, resulting in the formation of PEI-NUS hybrid nanosheet characterized by both high porosity and strong affinity to CO 2 . These nanosheets are assembled into ultrathin lamellar membranes with thicknesses ranging from 40 to 120 nm. The amines of PEI polymers significantly facilitate the CO 2 transfer as reaction carriers, resulting in a substantially improved CO 2 /N 2 separation performance with a CO 2 permeance of 410 GPU and a CO 2 /N 2 selectivity of 90, which are among the best for MOF membranes in CO 2 separation. This in-situ functionalization strategy paves the way for the fabrication of ultrathin 2D membranes for various separations.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2024
·
IF 2
Xiaodong Shen,Yinde Zhang,Yanxia Li,Long Shen,Jialin Shi,Yang Li
Phase equilibria of carbon dioxide (CO2) hydrate in aqueous solutions of N-methyldiethanolamine (MDEA) at four different mass fractions (5, 10, 15, and 25 wt %) in the temperature range of 274.01 to 281.93 K and pressure range of 1.79 to 4.34 MPa were experimentally investigated by adopting an isochoric pressure search method. The reliability and accuracy of our experimental apparatus and method were examined by comparing the measured data with published ones. The enthalpy of CO2 hydrate dissociation was calculated by the Clausius–Clapeyron equation. The experimental results showed that MDEA acted as a thermodynamic inhibitor which could suppress the equilibrium line of CO2 hydrate to lower temperatures or higher pressures. The thermodynamic inhibition effect was enhanced after increasing the mass fraction. However, it was weaker than the conventional thermodynamic inhibitors of ethylene glycol (EG) and sodium chloride (NaCl). MDEA had synergistic inhibition effects with EG and NaCl, as their mixtures had stronger thermodynamic inhibition performance. The average enthalpies of CO2 hydrate dissociation in the presence of MDEA (5 to 25 wt %) were found to be in the range of 67.562 to 80.776 kJ·mol–1, which were very close to that of pure water. The research results have theoretical guidance for the flow assurance of natural gases.
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Greenhouse Gases-Science and Technology
·
2024
·
IF 2.7
Lanxin Li,Zhibo Luo,Wei Zou,Shengke Liang,Hong Wang,Chen Zhang
Amine-functionalized porous polymers have been considered as a prominent chemical adsorption material for carbon capture and storage (CCS) process, because of their large adsorption capacity and high selectivity. By comparison, the low energy-consumption for desorption and high recyclability are the advantages of the physical adsorption approach. In this work, an amine-functionalized hierarchical porous polymer was prepared by HIPE (high internal phase emulsions) template and amine impregnation strategy, and applied as CO 2 adsorbent to realize chemical adsorption and physical adsorption simultaneously. First, a hierarchical porous matrix of poly(styrene-glycidyl methacrylate) was prepared by the HIPE method. The formed meso/micropores in the typical porous polymer matrix could attract CO 2 molecules, where the physical adsorption was achieved. Subsequently, PEI (polyethyleneimine) was impregnated into the porous polymer with abundant macropores, and the numerous of amino groups provided the reaction sites, where the chemical adsorption was achieved. As a result, an effective CO 2 adsorption material was obtained via controlling the porous structure by changing the volume fraction of dispersive phase, impregnation condition and amine loading. Aided by the chemical adsorption of amino groups, the CO 2 adsorption capacity of the obtained adsorbent reached 3.029 mmol/g. Moreover, the CO 2 adsorption thermodynamics confirmed the physicochemical synergistic adsorption, and then the Q st reduced to 31–42 kJ/mol and a good cyclic stability was obtained. As conclusion, the porous adsorbent showed a good industrial application prospect. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.
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ACS Omega
·
2024
·
IF 3.7
Liyuan Cai,Jingchun Wu,Miaoxin Zhang,Keliang Wang,Zhao Yang
Phase separation of microemulsions occupies a key position in many applications, such as oil recovery, nanomaterial synthesis, and chemical reactions. Achieving an intelligent response is crucial to microemulsion development and application. For this reason, in this study, CO2-responsive superamphiphilic molecules were developed as rapidly switchable oil-in-water microemulsions. These superhydrophilic molecules with linear structures were produced by electrostatic interaction of stearic acid and aminotrimethyltriazine COSM-1 in a 1:1 molar ratio. The introduction of n-butanol as a cosurfactant in the CO2-responsive microemulsion system resulted in the spontaneous formation of stable microemulsions. The effect of the addition of n-butanol on the carbon dioxide-responsive microemulsion system was investigated, and the optimum amount of n-butanol was determined by optimization. After exposure to CO2 for 30 s, the superhydrophilic molecules decomposed into inactive components at the interface, leading to a complete phase separation of the microemulsion into oil and water phases. The system was purged with N2 at 60 °C for 10 min to remove the CO2, and the phase separation system was transformed into a clear microemulsion, which was then evaluated for its properties. The rapid response and complete demulsification of these surface CNFS superamphiphiles to CO2 suggest that they have promising applications in product separation, microemulsion recovery, and enhanced crude oil recovery.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Minglu Li,Siyu Kuang,Yaxin Jin,Haoyuan Chi,Sheng Zhang,Xinbin Ma
Copper-based catalysts exhibit an excellent ability in producing C 2 chemicals during CO 2 RR. However, the unsustainable Faradic efficiency (FE) resulting from the reconstruction makes keeping catalyst behavior challengeable. In this study, we synthesized CuO nanosheets and incorporated a small amount of nickel on surface to improve the stability of nanosheets. By inhibiting the dissolution of Cu through the incorporation of Ni, our CuO + Ni-surface catalyst could achieve a double increase in stability compared to CuO nanosheets. Using a combination of electrochemistry, density functional theory calculations, in situ UV–vis spectrometer and inductively coupled plasma optical emission spectrometry, we elucidate the mechanisms behind the increased stability. The incorporation of Ni reduces the tendency of Cu oxidation at higher overpotential and strengthens the bonds between surface and subsurface Cu atoms. This work highlights a promising approach to enhance the stability and efficiency of copper-based catalysts in CO 2 RR, proposing the way for more sustainable catalytic processes.
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ENERGY & FUELS
·
2024
·
IF 5.2
Eunchae Oh,JeongA Kim,Jaewon Jang,Nodo Lee,Jaehoon Sah,Harok Jeong,Sang Won Lee,Dong Young Kim,Seung-Yeol Jeon,Byung-Joo Kim,Junghoon Yang,Jungpil Kim
Converting carbon dioxide (CO2) to carbon nanotubes (CNTs) is economically advantageous due to the high cost of CNTs. However, the one-step conversion of CO2 to CNTs compromises their quality owing to the oxidizing nature of CO2. We synthesized single-walled CNTs (SWCNTs) from CO2 via a two-step tandem process. CO2 was converted to methane (CH4) using a Ni/SiO2 catalyst with various Ni contents, achieving a CH4 selectivity of >96.0% at 300 °C on 30 wt % Ni/SiO2. Subsequently, CNTs were produced from the mixed gas consisting of 12.1% CH4, 4.2% CO2, 5.8% CO, 36.2% H2, and 41.7% carrier gas using Fe–Mo/MgO catalyst at temperatures of 700–900 °C. High-yield CNTs were produced from the mixed gas, as demonstrated by analysis of CH4 conversion rate and CNTs yield at different reaction temperatures. The temperature increase enhanced the CNTs crystallinity, reducing their diameter and the number of walls. Electrochemical diagnostic analysis reveals the synthesis of a higher proportion of SWCNTs at 900 °C. The proposed approach demonstrates a promising strategy for high-value CO2 utilization.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Qin Ding,Jianhua Lin,Xiaoyu Li,Yu Dong,Yongchun Bao,Huazhong Liang,Quan Zhuang,Jinghai Liu,Yin Wang
Carbon dioxide (CO 2 ) electroreduction to valuable chemicals is a promising approach for efficient carbon utilization. Herein, we propose an in situ electrochemical reconstruction method to regulate the selectivity of electroreduction of CO 2 into CO or HCOOH using a copper sulfide-loaded copper foam (Cu 2 S/CF) self-supporting electrode. Cu 2 S/CF under the applied potential of −0.2 V versus reversible hydrogen electrode (vs. RHE) maintain as the intial one, and Cu + are partially reduced to Cu 0 under the applied potential of −0.4 V vs. RHE forming vacancy S defects (V S ) in Cu 2 S. Notably, the Cu 2 S/CF achieve a potential regulable electroreduction CO 2 into CO with faradaic efficiency (FE) of 84.6 % at the applied potential of −0.2 V vs. reversible hydrogen electrode (RHE) and HCOOH with FE of 81.6 % at −0.4 V vs. RHE. Density functional theory (DFT) calculations reveal the different CO 2 adsorption configurations of catalytic centers resulting in the difference on the reduction products. Saturation Cu site on Cu 2 S surface favours to adsorb CO 2 with end-on configuration of *COOH for CO production, and unsaturation Cu site on Cu 2 S-V S surface prefers to the bridge configuration of *O*COH for HCOOH synthesis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Qiang Zheng,Zhenguo Liang,Derui Li,Fuxin Yang,Houzhang Tan,Xiaopo Wang
Deep eutectic solvent (DES) has the potential to replace aqueous amines for carbon capture. However, the reported DESs fail to absorb CO 2 equivalent to that absorbed by aqueous amines. To combine the excellent performance of amines and DESs, 9 amine-based DESs were prepared. The tetraethylammonium chloride was selected as the hydrogen bond acceptor, while ethanolamine, diethanol amine and triethanolamine were selected as the hydrogen bond donors. The molar ratios range from 1:4 to 1:6. Their properties were analyzed, including the structure, the thermal behavior and the potential corrosion. It has been determined that all DESs show a large liquid range (200 ∼ 600 K). Furthermore, the absorption characteristics of 9 DESs were studied. It has been found that the absorption capacity of DES3 and DES5 can reach up to 0.4066 and 0.3752 mol CO 2 /mol absorbent respectively, even 3 ∼ 6 times amount compared with the corresponding aqueous amines. At the laboratory level, the heat duty for the desorption process at 413.15 K of DES1 is 21.31 % of that for that of 30 wt% MEA at 393.15 K. For DES5, this value is 6.70 %. Besides, these DESs can maintain their splendid performance in absorption–desorption after 5 cycles. Meanwhile, the thermal stability and viscosity of the rich-absorbents were analyzed. Rich-absorbents are stable. Furthermore, effects of water have been inspected. The added water reduces the viscosity but confines the absorption capacity. For balance, the addition of 10 wt% water is recommended. Finally, the absorption mechanism was revealed. Both the physical and chemical absorption promote the absorption capacity of DESs.
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