APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Junya Wang,Chenxi Ma,Shikun Wen,Ping Ning,Yu Zhang,Yi Liu
This study synthesized a composite material of ZIF-67 and black titanium (BT) with high CO 2 reduction capability via a mechanochemical method. Through in-depth analysis of the morphology, structure, optical properties, and electrochemical behavior of the ZIF-67-BT composite photocatalyst, it was confirmed that the composite successfully formed an S-scheme heterojunction structure. This configuration can effectively separate photogenerated charge carriers, resulting in superior CO 2 reduction performance. The findings indicate that the composite material has optimal catalytic performance when the ZIF-67 doping content reaches 30 wt% (30 %ZIF-BT). Within 5 h, 30 %ZIF-BT exhibited excellent photocatalytic activity, with CO and H 2 yields reaching 2486.4 μmol·g −1 and 3495.0 μmol·g −1 , which were 44.0 and 29.4 times greater than the yields of BT, and 2.4 and 1.4 times than ZIF-67. The syngas (comprising CO and H 2 ) generated by ZIF-BT, with an adjustable CO to H 2 ratio ranging from 1:1.40 to 1:2.47, is regarded as a significantly beneficial and crucial intermediate for further conversion into valuable hydrocarbon fuels via Fischer-Tropsch synthesis. This research offers a feasible method to construct S-scheme heterojunction in ZIF-BT composite materials.
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JOURNAL OF CATALYSIS
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2025
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IF 6.5
Ziyang Xu,Liang Chen,Chunbo Wang
Reaching high activity over Ni-based catalysts for CO 2 methanation at lower temperature remains a critical challenge. Herein, a surface hydroxylation strategy was developed to enhance the catalytic performance of Ni catalysts under mild conditions. By treating γ-Al 2 O 3 with H 2 O 2 solutions of varying concentrations, the surface hydroxyl (–OH) group density was effectively tuned. Catalytic evaluations revealed that hydroxylation of the support significantly enhances CO 2 methanation performance. Among the series, Ni/A-OH-6 exhibited the highest activity, achieving a turnover frequency (TOF) of 2.129 h −1 at 240 °C, approximately eight times higher than that of the unmodified Ni/A catalyst (0.266 h −1 ), thereby demonstrating a remarkable enhancement in intrinsic activity. Comprehensive characterizations demonstrated that surface –OH significantly enhanced CO 2 adsorption via the formation of HCO 3 * species. In situ DRIFTS studies further confirmed that hydroxyl-induced HCO 3 * species convert more readily to HCOO*, facilitating the hydrogenation pathway and thus contributing to the improved low-temperature activity. This work highlights surface hydroxyl engineering as a simple yet effective approach to boost catalytic efficiency, delivering guidance for the rational development of high-efficiency CO 2 utilization catalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Shaojun Jia,Jin Huang,Yuqing Wang,Wu Chen,Yao Jiang,Peng Cui
Nonaqueous liquid–liquid CO2 phase change absorbents (CPCAs) have garnered significant attention due to their potential for efficient and energy-saving CO2 capture in the amine-scrubbing process. This study introduces a novel nonaqueous CPCA that utilizes aminoethylethanolamine (AEEA) as the main amine absorbent, dimethyl sulfoxide (DMSO) as the organic solvent, and N-ethylmorpholine (NEM) as the phase separator. To mitigate the high viscosity of the rich phase in CPCA, diethanolamine (DEA) is introduced as a viscosity regulator, which reduces the viscosity by 79.3% by weakening the intermolecular hydrogen bonding in the CO2 products. Notably, the optimized CPCA of A20E10D40N30 demonstrates a high cyclic capacity of 2.94 mol·kg–1 and a low regeneration energy consumption of 1.79 GJ·t–1 of CO2. Overall, the efficient CO2 capture performance, low regeneration energy consumption, and minimal corrosivity make this CPCA a promising candidate for industrial CO2 capture applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Xin-Ran Shi,Sai-Nan Guo,Ruoxi Zhang,Biao Yang,Hua Zou,Jie-Xin Wang
Metal–organic frameworks (MOFs) have emerged as pivotal materials for the photocatalytic reduction of CO2 to CO due to their exceptionally high surface areas and abundant active sites. However, most of the currently reported MOFs are confined to micropores (<2 nm), which limits adsorption/desorption and substance transport during photocatalytic CO2 reduction reactions. Herein, hierarchically porous MOFs (HP-MOF-74) were synthesized based on the assembly of MOF-74-Ni nanoparticles with different particle sizes (21, 42, and 85 nm) using spray-drying technology. The simultaneous enhancement of CO2 adsorption performance and photoelectroactivity was achieved in HP-MOF-74 due to the additional mesoporous structure formed by the nanoparticle stacking. The HP-MOF-74 exhibits 1.14–1.38 times improvement in the CO2 adsorption capacity compared to the corresponding initial MOF-74 nanoparticles (N-MOF-74). Meanwhile, the hierarchical architecture enhances photon utilization through improved light reflections and accelerates electronic transmission via additional mesopore pathways. These synergistic advantages collectively contribute to a 1.2–2.1 times enhancement in the CO generation rates of HP-MOF-74 compared with N-MOF-74 counterparts. Particularly, HP-MOF-74–42 nm demonstrated the highest CO production rate of 6.65 μmol h–1, outperforming most reported MOF-based photocatalysts. The construction of hierarchically porous MOFs provides a new idea for the design of highly efficient CO2 reduction photocatalysts.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Feng Xie,Shaoqi Zhan,Zihan You,Jiao Lan,Linghu Meng,Wei Zheng,Yuanguo Chen,Ming Peng,Yongwen Tan
Electrochemical reduction of CO 2 , a technology with great potential for renewable energy storage and climate change mitigation, depends on critical C─C coupling steps in CO 2 RR to ensure efficient high-value hydrocarbon production. In this work, a local interface electric field and a tip-induced electric field are constructed on Ag-embedded Cu nanoneedle arrays to enhance the concentration of the *CO intermediate and regulate the adsorption of key intermediates, respectively. This optimization of the reaction microenvironment promotes the deep reduction of the *CO intermediate into multi-carbon products (C 2+ ), with a faradaic efficiency of 83.7% and a C 2+ local current density of −526 mA cm −2 within gas-fed flow cells. Experimental evidence and simulations validate that the interface electric field of the Cu-Ag bimetallic catalyst increased surface *CO coverage, substantially lowering the formation barrier for *CHO intermediate, and the tip-induced electric field that can stabilize *CO intermediate and suppress hydrogen evolution, promoting the C─C coupling process. The formation of the dual electric fields profoundly induced local environments and ultimately, the dominant C 2+ product, which offers significant design guidelines for adjusting the supply and demand balance of reaction intermediates.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Wanting Zhang,Jiawei Ruan,Xinzi Wu,Qian Liu,Kunchi Xie,Lifang Chen,Zhiwen Qi
The transformation of captured CO 2 into highly-valued dimethyl carbonate (DMC) is a promising approach for CO 2 capture and utilization. However, the direct synthesis of DMC from CO 2 and methanol is limited by high activation barrier derived from inert CO 2 and thermodynamic equilibrium constraints. Herein, three 1-butyl-1-methylpyrrolidinium (BMP)-based ionic liquid (ILs) with polar pyrrole, pyrazole, and 1,2,4-triazole (Tz) azole anions were designed to integrate CO 2 absorption and transformation into DMC. [BMP][Tz] exhibits a relatively high CO 2 uptake capacity of 0.6 mol·mol IL −1 and DMC yield reaches 12.2 % under mild reaction conditions of atmospheric temperature and pressure in 12 h. The reaction equilibrium thermodynamic model reveals that the process involves a combination of 1:1 and 2:1 stoichiometric reaction between [BMP][Tz] and CO 2 . Density functional theory calculations verify that [BMP][Tz] with increased absorption efficiency of azole anions promotes critical bond activation (particular C − O and O − H bonds), thereby enhancing catalytic efficiency. Besides, the reaction mechanism is clarified by the calculation of intermediates and transition state, wherein [BMP][Tz] can efficiently decrease the energy barrier of the rate-controlled step, which involves the insertion of CH 3 O − into CH 3 OCOO − species. Furthermore, polarity-induced phase separation of DMC from the IL phase to solvent phase favors DMC generation by breaking through the reaction equilibrium. The integration of CO 2 absorption-reaction-extraction based on basic and polar ILs, provides a promising approach for CO 2 capture and utilization.
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Industrial Chemistry & Materials
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2025
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IF 11.9
Shenzhen Cong,Si Sun,YiJing Zhang,Ming Wang,Zhehua Jia,Jiaoyu Peng,Huan Pang
Metal-organic framework (MOF) membranes have received widespread research attention as a novel membrane material for H2/CO2 separation. The preparation of MOF membranes can be extended by constructing MOF membranes with homogeneous heterogeneous structure and the MOF membranes with high permeance and high selectivity can be prepared. Here, we use the chelation-assisted interfacial growth process to construct a seeding layer, and then prepare Co-Zn-ZIF-L membranes with homogeneous heterogeneous structure by secondary growth for the efficient separation of H2/CO2. The resulting Co-Zn-ZIF-L membranes show an H2 permeances of 2156 GPU and the H2/CO2 selectivity of 31.6 at 298K and 1.0 bar, surpassing the Robeson upper bond (2008). Furthermore, the Co-Zn-ZIF-L membrane has a H2/CO2 separation stability of 65 h and can efficiently separate to obtain pure H2.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
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IF 3.7
Wei Liu,Xiaoshen Li,Shaohui Xiong,Xueyang Jiang,Jiayan Yan,Xiang Duan,Yingtian Zhang,Qingpeng Cheng,Ye Tian,Xingang Li
CO 2 hydrogenation to methanol is a critical technology for hydrogen energy conversion and a promising approach to mitigate the energy crisis and greenhouse effect. However, developing highly selective catalysts remains a major challenge for its practical application. Herein, we synthesize an efficient CoCuInO-r catalyst with Cu 11 In 9 and Co 0 dual sites on In 2 O 3 via a sol-gel method. The Cu 11 In 9 intermetallic compound enhances H 2 adsorption capacity and strength, and increases oxygen vacancy concentration on the catalyst surface, thereby improving CO 2 activation and hydrogenation efficiency. Meanwhile, Co 0 suppresses the desorption of the *CO species, facilitating its further hydrogenation to methanol. In-situ DRIFTS experiments indicate that the CO 2 hydrogenation to methanol over CoCuInO-r follows the formate pathway. Compared with CuInO-r (containing Cu 11 In 9 on In 2 O 3 ), CoCuInO-r exhibits a ∼20% increase in methanol selectivity and a 2-fold higher methanol space-time yield, reaching 7.68 mmol·g cat -1 ·h -1 at 300 °C and 4 MPa.
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JOURNAL OF THE INDIAN CHEMICAL SOCIETY
·
2025
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IF 3.4
Wei Shen,Zilong Yang,Xiaolin Guo,Hongxiao Jin,Wenxiang Chai,Hongliang Ge,Dingfeng Jin
Amino acid ionic liquids (AAILs) are potential green substitutes of aqueous amine solutions for carbon dioxide (CO 2 ) capture. In this study, we prepared three amino acid ionic liquids, constructed from tetrabutylphosphine hydroxide in combination with glycine, histidine, and arginine. We have conducted a comprehensive study on the CO 2 absorption capacity of structures containing single, double, and triple N–H groups. The solubility of CO 2 in [P 4444 ][Gly], [P 4444 ][His] and [P 4444 ][Arg] were measured experimentally over a temperature range of 30–110 °C and up to a pressure of 0.75 MPa. The results indicate that the solubility of carbon dioxide in amino acid ionic liquids decreases with increasing temperature, while it increases with increasing pressure. The optimal CO 2 absorption conditions of three amino acid ionic liquids were determined to be 50 °C, 0.75 MPa. Moreover, CO 2 absorption capacity of three amino acid ionic liquids followed the order: [P 4444 ][Arg] > [P 4444 ][His] > [P 4444 ][Gly]. Studies on the recycling and regeneration of amino acid ionic liquids verified their reusability in the process and confirmed that the reaction between AAILs and CO 2 could be reversed at 140 °C. Finally, the recycle capacity and CO 2 removal efficiency of [P 4444 ][Gly], [P 4444 ][His] and [P 4444 ][Arg] were evaluated.
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ChemistrySelect
·
2025
·Vol. 10
·期 32
·e03728
·
IF 2
Yong Rui Wang,Su Dan Bao,Agula Bao,Zheng Ming Li,Bodeligeteng Huang
Graphical This study develops nitrogen-enriched porous carbon materials using chitosan and g-C 3 N 5 through hydrothermal carbonization and pyrolysis. The optimized adsorbent (S200-6) exhibits a high CO 2 adsorption capacity (3.98 mmol/g at 298 K, 1 bar), large specific surface area (2306 m 2 /g), and excellent selectivity (14.3 for CO 2 /N 2 ). Carbon capture and storage are crucial because of the environmental issues caused by excessive CO 2 emissions. Porous carbon is considered the most promising adsorbent. The precise adjustment of the pore structure and surface active sites of samples is necessary to increase their CO 2 adsorption capacity. In this study, chitosan-based N-doped porous carbon materials were developed using g-C 3 N 5 as the self-sacrificial templating agent and N dopant, respectively, via hydrothermal and pyrolytic activation methods. CO 2 adsorbents possessing a large specific surface area (2084–2450 m 2 /g), microporous structure, and N content were synthesized by varying the hydrothermal temperature and g-C 3 N 5 ratio. The maximum CO 2 adsorption capacity of the highest-performing adsorbent S200-6 was 3.98 mmol/g at 298 K and 1 bar. After 10 CO 2 adsorption and desorption cycles, S200-6 retained 94% of its initial adsorption capacity, indicating its excellent reusable stability. This study demonstrates the feasible preparation of porous carbon materials through a combination of g-C 3 N 5 with hydrothermal and pyrolytic activation methods and reveals the application potential of S200-6 as a CO 2 adsorbent.
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Frontiers in Bioengineering and Biotechnology
·
2025
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IF 4.8
Zhan Hu,Dantong Wang,Pengcheng Li,Yaoqi Hou,Guanyi Chen,Chunfeng Song
The CO 2 chemical absorption and microalgae conversion (CAMC) system can achieve low-energy consumption CO 2 capture and resource utilization, but the study on enhancing the synthesis of high-value products has been overlooked. In this study, the coupling strategy of nitrogen stress and exogenous phytohormones was applied to induce high-value products accumulation of Dunaliella salina in CAMC system, and the potential mechanism was also discussed. The results showed that phytohormones could promote D. salina growth by alleviating the oxidative damage under nitrogen limited treatment, especially in gibberellin (GA) group, and the biomass increased by 10.24%. In addition, phytohormones combined nitrogen limited changed carbon flow, directing more carbon to polysaccharose synthesis, supplementation with GA under nitrogen-limited conditions resulted in a 1.65-fold increase in polysaccharide content in D. salina compared to the control. Furthermore, supplementation with GA under nitrogen-limited conditions enhanced the accumulation of β-carotene, and the β-carotene yield and content were 18.52% and 14.46% higher than control. This study suggested that GA could further affect carbon metabolism and products synthesis of D. salina under nitrogen stress, and provided a possible insight in improving the production of economical metabolites in CAMC system.
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PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Zhu Jiawei,Zhang Yu,Chen Zitao,Zhang Zhenbao,Tian Xuezeng,Huang Minghua,Bai Xuedong,Wang Xue,Zhu Yongfa,Jiang Heqing
Cu-oxide-based catalysts are promising for CO 2 electroreduction (CO 2 RR) to CH 4 , but suffer from inevitable reduction (to metallic Cu) and uncontrollable structural collapse. Here we report Cu-based rock-salt-ordered double perovskite oxides with superexchange-stabilized long-distance Cu sites for efficient and stable CO 2 -to-CH 4 conversion. For the proof-of-concept catalyst of Sr 2 CuWO 6 , its corner-linked CuO 6 and WO 6 octahedral motifs alternate in all three crystallographic dimensions, creating sufficiently long Cu-Cu distances (at least 5.4 Å) and introducing marked superexchange interaction mainly manifested by O-anion-mediated electron transfer (from Cu to W sites). In CO 2 RR, the Sr 2 CuWO 6 exhibits significant improvements (up to 14.1 folds) in activity and selectivity for CH 4 , together with well boosted stability, relative to a physical-mixture counterpart of CuO/WO 3 . Moreover, the Sr 2 CuWO 6 is the most effective Cu-based-perovskite catalyst for CO 2 methanation, achieving a remarkable selectivity of 73.1% at 400 mA cm −2 for CH 4 . Our experiments and theoretical calculations highlight the long Cu-Cu distances promoting *CO hydrogenation and the superexchange interaction stabilizing Cu sites as responsible for the superb performance.
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