CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Qiang Li,Yuhang Ding,Teng Wang,Zhuo Xiong,Junying Zhang,Yongchun Zhao
Dual-function amine-based electrolytes provide both carbon dioxide (CO 2 ) capture and electrocatalytic CO 2 reduction capabilities, combining the capture and conversion steps of conventional separations in a single system, increasing efficiency and reducing energy consumption. Cations serve as critical constituents within bifunctional amine-based electrolytes, integral to both CO 2 absorption mechanisms and the electrochemical reduction of carbamates, but this issue has not been comprehensive studied. In this study, we investigated the effect of five different cations (M + = Li + 、Na + 、K + 、Rb + 、Cs + ) on the CO 2 capture and electroreduction properties of dual-function amine-based electrolyte. Electrochemical comparative analyses reveal that the presence of larger cations (Cs + ) significantly reduces series resistance and charge-transfer resistance, while augmenting electric double-layer capacitance and electrochemical surface area. These synergistic effects culminate in elevated current densities and accelerated reaction rates during carbamate reduction processes. Density functional theory (DFT) simulations elucidate that expanding cationic radii strengthen both adsorption trends and charge transfer of carbamate (R 1 R 2 NCOO - ) at electrode–electrolyte interface. Comparative analysis of the HOMO-LUMO orbitals shows that R 1 R 2 NCOO - Cs + is more easily reduced and electronic excited. These computational validate the observed enhancements in current density from experimental electrochemical. Higher electrolyte concentrations (≥1 M) enhance the selectivity of carbamate reduction but impede mass transfer due to increased viscosity following CO 2 absorption. Conversely, lower electrolyte concentrations (<1 M) improve the current density of carbamate reduction but reducing CO 2 capture rates. Moreover, an equimolar cation-to-amine optimizes the enhancement of CO 2 absorption capacity and electroreduction efficiency. This work provides a comprehensive understanding of how cations influence the electrocatalytic reduction of captured CO 2 in amine-rich solutions, offering valuable insights for the design of electrolytes for CO 2 capture and electroreduction.
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Journal of CO2 Utilization
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2024
·
IF 7.2
Xinjuan Li,Yan Liu,Ao Li,Xuening Ma,Xianbin Jia,Yahao Dong
Constructing stable nanochannels and nanoconfined environments for ionic liquids holds significant application value in gas separation, ion channels, and related fields. The functional polyionic liquid synthesized in this study exhibits a controllable assembly structure and demonstrates liquid crystal properties. Through heating and water treatment, the polyionic liquids crosslink to form multi-hierarchical nanopores, including sub-nanochannels with pore sizes similar to CO 2 , without the need for a catalyst. The specific surface area and pore size of the polyionic liquid network (PILC) were adjusted by regulating the self-assembly of polyionic liquids in water. The unique PILC, combining ionic liquid nanopores and liquid crystal structure properties, shows high CO 2 adsorption performance and excellent CO 2 /N 2 selectivities, surpassing commonly reported ionic liquid porous materials. Furthermore, PILC-2 exhibits good catalytic performance for CO 2 cycloaddition, and its catalytic activity and selectivity did not significantly decrease after five cycles. This study successfully introduces hierarchical ionic liquid nanochannels into porous networks without involving any inorganic ordered nanomaterials. This provides a simple and effective approach for the highly selective adsorption and separation of CO 2 , as well as for the preparation of catalytic materials.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Xiaoqiang Wang,Menghan Li,Zhiyuan Liu,Zhuang Shi,Daoyong Yu,Baosheng Ge,Fang Huang
Utilizing carbonic anhydrase (CA) to catalyze CO 2 hydration offers a sustainable and potent approach for carbon capture and utilization. To enhance CA's reusability and stability for successful industrial applications, enzyme immobilization is essential. In this study, delignified bamboo cellulose served as a renewable porous scaffold for immobilizing CA through oxidation-induced cellulose aldehydation followed by Schiff base linkage. The catalytic performance of the resulting immobilized CA was evaluated using both p -NPA hydrolysis and CO 2 hydration models. Compared to free CA, immobilization onto the bamboo scaffold increased CA's optimal temperature and pH to approximately 45 °C and 9.0, respectively. Post-immobilization, CA activity demonstrated effective retention (>60 %), with larger scaffold sizes (i.e., 8 mm diameter and 5 mm height) positively impacting this aspect, even surpassing the activity of free CA. Furthermore, immobilized CA exhibited sustained reusability and high stability under thermal treatment and pH fluctuation, retaining >80 % activity even after 5 catalytic cycles. When introduced to microalgae culture, the immobilized CA improved biomass production by ∼16 %, accompanied by enhanced synthesis of essential biomolecules in microalgae. Collectively, the facile and green construction of immobilized CA onto bamboo cellulose block demonstrates great potential for the development of various CA-catalyzed CO 2 conversion and utilization technologies.
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AICHE JOURNAL
·
2025
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IF 4
Xinrui Liu,De Ao,Mao Ye,Zhi Wang,Zhihua Qiao,Song Zhao
Metal–organic framework (MOF) glass holds great promise for gas separation applications. However, the inherent low porosity of MOF glass poses a considerable challenge in improving membrane permeability. In this work, a self-supporting MOF crystal-glass composite (CGC) membrane was synthesized via an innovative blending and melting approach, in which ZIF-62 powder was converted into an amorphous glassy phase and ZIF-9 powder was partially flux-melted, effectively preventing the reorganization of Zn─N bonds within ZIF-62. Consequently, the composite component structure significantly enhances the porosity and permeability of the MOF glass membrane. Furthermore, the incorporation of cobalt into the membrane matrix has notably enhanced its adsorption affinity for CO 2 , thereby boosting CO 2 /CH 4 selectivity. The resultant a g [(ZIF-9) 0.2 /(ZIF-62) 0.8 ] membrane has demonstrated exceptional CO 2 permeability of 20,324 barrer and superior CO 2 /CH 4 selectivity, both surpassing the 2018 upper bound. Thus, the innovative strategy for the design of MOF CGC membranes offers effective solutions to the challenges inherent in gas separation processes.
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Industrial Chemistry & Materials
·
2025
·
IF 11.9
Longlong Wang,Ruirui Wang,Shuang Wei,Kexin Li,Hasnain Nawaz,bin He,Mengyue Li,Ruixia Liu
Photothermal synergistic catalysis significantly enhances the efficiency of photocatalytic CO2 reduction, offering a promising strategy for accelerated CO2 resource utilization. Herein, a series of CuxInyS photocatalysts were synthesized, exhibiting tunable band gap energy by varying the Cu/In/S atomic ratios for photothermocatalytic CO2 conversion to C2H4. The typical CuInS2 demonstrates a more negative conduction band, significantly enhancing electron reduction ability and facilitating the multi-electron reduction of CO2 to C2H4. Additionally, the high sulfur vacancy in CuInS2 generates additional active sites, enhances charge separation efficiency, and consequently improves catalytic activity. The generation rate of ethylene reaches 45.7 μmol·g-1·h-1 with the selectivity of 79.7%. This study provides a new avenue for producing ethylene in photothermal catalysis, as well as highlights the superiorities of CuInS2 catalyst.
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Nature Communications
·
2025
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IF 15.7
Qian Zhengyi,Han Guokang,Tan Yingjun,Ye Na,Wang Shuguang,Lin Zheng,Huang Qizheng,Gu Yu,Guo Hongyu,Liu Fei,Wang Kai,Li Lu,Shang Changshuai,Luo Mingchuan,Guo Shaojun
Copper-based catalysts are the premier choice for electrochemical reduction of CO 2 (CO 2 RR) into hydrocarbons or oxygenates. However, the facilely structural reconstruction of copper sites during electrolysis poses significant challenges to the long-life electrolytic efficiency. Herein, we leverage the strong σ-π dative bonding between Cu δ+ and alkyne-based ligands to stabilize copper sites for the prolonged CO 2 RR. We demonstrate the feasibility of taming the electronic structures of copper sites through the tug of war between σ and π backbonding interactions. The optimal copper organic polymer with methoxy group functionalization (OMe-PhCu) exhibits a moderate charge density of copper sites and an intensified local asymmetric charge distribution of coordinative carbon, enhancing the selectivity of methane with a Faradaic efficiency of 68.8% and a partial current density of 324.5 mA cm −2 in acidic electrolyte. In situ spectra and density functional theory calculations reveal enhanced *CO adsorption and lowered energy barrier for CO 2 RR into methane over OMe-PhCu. Building upon such stable Cu δ+ sites, we further construct Cu δ+ /Cu 0 catalytic interfaces for the generally enhanced electrosynthesis of multi-carbons and ammonias. This synthetic chemistry paves the pathway for the design of stable catalytic active sites for renewable conversions.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120640
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IF 7.2
Yifan Wang,Zeliang Xiong,Shilin Xu,Yuan Gao,Haoli Zhou,Wanqin Jin
Polyimides with intrinsic microporosity are promising materials for gas separation, but their industrial application is hindered by poor long-term stability. This study proposes diamine modification of a polyimide membrane with diamines, such as p-phenylenediamine (p-PD), to enhance both membrane stability and selectivity for separating gas pairs such as CO 2 /CH 4 . Various characterization techniques confirmed the crosslinking reaction between the diamine and imide groups, which restricted the movement or rearrangement of polymer chains, resulting in improved membrane anti-plasticization performance and stability. Meanwhile, CO 2 -philic emeraldine base and quinone structures were formed due to the in-situ oxidation of p-PD during the crosslinking process, which significantly boosted CO 2 /CH 4 selectivity. The maximum selectivity (44.5), which is 66.0 % higher than that of the pristine membrane, was achieved using a p-PD-modified polyimide membrane for the separation of pure single CO 2 /CH 4 . Additionally, the separation of other gas pairs (such as CO 2 /N 2 ) and the effect of pressure on the separation of a CO 2 /CH 4 mixture were investigated using the p-PD-modified polyimide membrane, which demonstrated improved performance. Thus, this study provides a reference for enhancing the selectivity and stability of polyimide membranes through diamine modification using p-PD and its analogues.
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CHEMISTRY OF MATERIALS
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2025
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IF 7
Jiangquan Lv,Yin Gao,Hanyang Liu,Zimin Han,Guoqing Feng,Rui Yang
Renewable-powered electrochemical CO2 reduction (ECO2R) provides a sustainable route to convert CO2 into valuable fuels and chemicals. However, conventional ECO2R systems face high energy costs due to the sluggish oxygen evolution reaction (OER) at the anode. Replacing the OER with biomass electrooxidation (e.g., glycerol oxidation reaction, GOR) can lower energy consumption while coproducing high-value chemicals. However, the construction of an efficient and cost-effective bifunctional catalyst remains a challenge. Herein, we design a low-cost, bifunctional Ni12P5@NCNT catalyst with a bamboo-like nanotube morphology for coupled ECO2R and GOR. The Ni12P5@NCNT exhibits exceptional performance, achieving 82% CO selectivity at −0.7 V vs RHE in ECO2R and a 95% Faradaic efficiency for formate production in GOR. The integrated system significantly reduces overpotential (219 mV) compared to conventional ECO2R //OER setups. Experiments reveal that the strong electronic interaction between Ni12P5 and NCNT enhances the CO2/glycerol adsorption and accelerates charge transfer, boosting both ECO2R and GOR activity. This work provides a promising strategy for co-upgrading CO2 and glycerol into valuable products using nonprecious metal catalysts.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2025
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IF 3.7
Jianjian Yi,Tiaolong Lv,Guoxiang Zhang,Xu Wang,Xianglin Zhu,Yubo Zhou,Li Li,Xingwang Zhu,Xiaozhi Wang
Amorphous/crystalline catalysts can effectively integrate the advantages of both phases, overcoming the low active site density in crystalline phases and the poor charge separation in amorphous ones. In this work, we report an alkali salt-assisted partial phase transition strategy to synthesize amorphous/crystalline CoMnO x -400 nanosheets for photocatalytic CO 2 reduction. As a result, the as-prepared CoMnO x -400 demonstrates superior CO production performance (146.09 µmol g −1 h −1 , 93.6% selectivity), significantly outperforming amorphous CoMnO x -260 (66.65 µmol g −1 h −1 ) and crystalline CoMnO x -500 (89.52 µmol g −1 h −1 ). Supported by systematic characterizations, we propose that the high efficiency of CoMnO x -400 is attributed to two factors: (i) the charge migration between amorphous and crystalline phases across the seamless contact interface can enhance charge separation efficiency, and (ii) the amorphous domains can provide abundant surface defective active sites for CO 2 adsorption and activation. This work highlights the critical role of phase engineering, particularly the construction of amorphous/crystalline structures, in advancing solar-driven catalytic applications. Graphical This work presents an alkali salt-assisted annealing method to precisely synthesize CoMnO x with tunable crystallinity and systematically elucidating the structure-activity dependency between crystallinity and CO 2 photoreduction performance.
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ACS Catalysis
·
2025
·
IF 13.1
Yang Chen,Diwen Zhou,Yongli Chang,Yunzhao Xu,Hongqiao Lin,Lizhi Wu,Yu Tang,Chengyi Dai,Xingang Li,Lisheng Guo,Ting Qiu,Li Tan
The utilization of Rh-based catalysts in the direct production of ethanol from CO2 has been a subject of significant interest. However, to date, the precise active sites responsible for ethanol generation and the C–C coupling mechanism remain elusive. In this study, we present a Rh-based catalyst featuring nanoscale Rh–Fe alloy sites, which achieved an ethanol selectivity of 49.1% among all hydrocarbon and oxygenate products (CO excluded) under relatively mild reaction conditions (3.0 MPa, 200 °C, with a low metal loading of ≤1 wt %). The formation of ethanol proceeds via the HCOO* pathway with a CO insertion mechanism occurring at the alloy sites with a specific cluster size, where CH2* and CO* act as the crucial intermediates for C–C coupling. The electron interaction within the Rh–Fe alloy sites effectively reduces the energy barrier for the formation of the CH2CO* intermediate, thereby facilitating the production of ethanol. In contrast to the Rh–Fe alloy sites, the geminal-dicarbonyl binding configuration of CO* intermediates on Rh single sites favors the generation of byproducts such as methane and methanol, rather than ethanol. This research offers insights into the active sites and reaction mechanism of hydrogenation of CO2 to ethanol, thus enhancing the efficient utilization of Rh-based catalysts.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2025
·
IF 3.9
Pengchao Zang,Daokuan Liang,Jiyun Tang,Xiaozhe Wang,Lin Cui,Pei Zhao,Ning Qin,Zeyad Ammar Almutairi,Yong Dong
Adsorbents prepared by impregnating tetraethylenepentamine (TEPA) into porous materials represent promising candidates for CO 2 capture from coal-fired flue gas. This study impregnated TEPA into four types of resins to investigate the influence of different resins on the CO 2 adsorption performance of TEPA-resin adsorbents. Experimental data indicate that the CO 2 adsorption performance of TEPA-resin composites follows the order: DA201D > XAD-2 > ADS-17 > AB-8, where TEPA@DA201D exhibited the highest adsorption capacity of 3.46 mmol/g under 35℃ and 15 vol% CO 2 conditions. TEPA@DA201D possesses a hierarchical mesoporous structure with a high pore volume (1.084 cm 3 /g) and large average pore diameter (20.0 nm), which synergistically enhances CO 2 adsorption by promoting CO 2 diffusion and improving the dispersion of active sites. Simultaneously, SEM images reveal that DA201D exhibits the least aggregation of surface amine groups compared to other adsorbents. Different adsorption kinetic models reveal that its adsorption behavior conforms to the Avrami model, primarily governed by the synergistic effects of physical and chemical adsorption. The rate-limiting steps for CO 2 adsorption by the TEPA@DA201D adsorbent are mainly membrane diffusion and intra-particle diffusion at different temperatures. Furthermore, multifactorial interaction analysis indicates that adsorption temperature, gas flow rate, and CO 2 concentration independently regulate the adsorption capacity of TEPA@DA201D. This work provides theoretical guidance and design strategies for improving the design and performance of organic amine-modified resin-based adsorbents.
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Nanomaterials
·
2025
·Vol. 15
·期 24
·1903
·
IF 4.3
Reshalaiti Hailili,Yiming Gan
The development of versatile photocatalysts is crucial for comprehensive solutions to the intertwined challenges of the energy crisis and environmental pollution. This study presents a novel Bi3TiNbO9/Bi2MoO6(BTNO/BMO) heterojunction fabricated via a solvothermal method. Advanced characterization techniques verified the successful synthesis of the as-integrated BTNO/BMO heterostructure. The BTNO/BMO composite exhibited superior performance in multiple applications: efficient degradation of tetracycline reaching 90.2%, removal of gaseous nitric oxide (NO), and photocatalytic reduction of carbon dioxide (CO2) to carbon monoxide (CO) with a yield of 51.3 μmol·g−1. The constructed Type-II heterojunction demonstrated a remarkable ability to suppress charge recombination, thereby significantly enhancing the photocatalytic activity. This work highlights the dual-functional capability of the BTNO/BMO heterojunction for simultaneous environmental purification and fuel production, providing a promising material platform and a strategic design concept for sustainable technological development.
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