MOLECULES
·
2026
·Vol. 31
·期 13
·2332
·
IF 5.1
Renkun Huang,Haohao Yan,Runling Huang,Chen Zhou,Qiuzhong Li,Lu Chen,Ruowen Liang
A novel composite catalyst for photothermal CO2cycloaddition was developed by integrating the ionic liquid 1-ethylpyridinium bromide (EPB) with a copper-based metal–organic framework (HKUST-1). HKUST-1 was synthesized via a hydrothermal method and functionalized with EPB through a wet impregnation strategy to enhance its catalytic performance. Under xenon lamp irradiation and optimized conditions (80 °C, 1 MPa CO2pressure, 12 h, and 0.07% mol of TBAB bromide as a co-catalyst), the HK@EPB composite exhibited outstanding performance in catalyzing the conversion of CO2and various epoxides into cyclic carbonates. The exceptional catalytic activity arises from a synergistic multicomponent mechanism: the incorporation of EPB not only enhances CO2adsorption capacity but also provides photothermal energy for the reaction; simultaneously, EPB dissociates bromide ions to effectively initiate epoxide ring-opening. In particular, propylene oxide achieved a selectivity of 95% for the desired cyclic carbonate, surpassing most previously reported MOF-based catalysts. This system enables efficient catalysis under mild conditions through the synergistic contributions of the high CO2adsorption capacity and Cu2+/Cu+redox-mediated electron transfer of HKUST-1, the provision of nucleophilic Br-species from EPB to promote epoxide ring-opening, and the cooperative effect of TBAB. This study demonstrates that ionic-liquid-functionalized MOF composites can serve as sustainable and versatile catalytic platforms, offering an environmentally friendly pathway for large-scale CO2utilization.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123910
·
IF 7.5
Wenhao Hou,Jiaqi Xing,Lina Qiao,Yun Ju,Yaqi Liu,Jing He,Wenwen Wei,Jie Jiang,Hong Zhang
Water microdroplets possess energetic interfaces that can promote the reduction and utilization of carbon dioxide (CO 2 ). However, the mechanism by which acidity modulates CO 2 interfacial reactions in microdroplets remains unclear. Herein, CO 2 fixation in pyruvate-containing microdroplets was investigated over a pH range of 1.5–10.1. Online mass spectrometry showed that acidic conditions significantly enhance the reaction between CO 2 and pyruvate, particularly in smaller droplets and at lower pyruvate concentrations. A similar promotion was observed for another α-keto acid, α-ketoglutaric acid. Mechanistic analysis suggests that electrostatic attraction between interfacial anions (Cl - and OH - ) and protons amplifies the interfacial electric field at the air-water interface, which drives CO 2 fixation rather than conventional proton catalysis. These findings highlight the critical role of acidity in interfacial CO 2 -related chemistry and may help improve the understanding of environmentally relevant microdroplet carbon processes.
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Nature Communications
·
2026
·
IF 18.1
Ni Sulin,Xia Dong,Chen Can,Qiu Cheng,Li Youzhi,Yang Bin,Hou Yang,Lei Lecheng,Mao Zhengwei,Li Zhongjian
A hybrid system combining water electrolysis and H 2 autotrophic microorganism enables sustainable CO 2 valorization, but is hindered by low H 2 bioavailability and sluggish hydrogenase kinetics. Here, we report an interface-engineered inorganic–biological biohybrid, constructed by covalently anchoring iron single-atom catalysts (ISA) onto Cupriavidus necator ( C.N @ISA) via click chemistry. The ISA anchored interface generates a localized H 2 -rich microenvironment, accelerates H 2 dissociation, while the synergy between ISA and polyethylene glycol-phenylboronate linker stabilizes the inorganic-biological hybrid interface and promotes electron/proton transfer across microbial membrane. These coupled effects boost reduced form of nicotinamide adenine dinucleotide (NADH) regeneration and adenosine triphosphate (ATP) synthesis. In addition, ISA exhibits nanozyme-like activity, scavenging reactive oxygen species to protect cell viability. As a result, C.N @ISA achieves CO 2 -to-bioplastic poly- β -hydroxybutyrate production of 1058.8 mg L −1 with a Faradaic efficiency of 42.0%. Integrating theoretical calculations, electrochemical analysis, and transcriptomics confirms that ISA simultaneously enriches and activates H 2 while reinforcing intracellular metabolism, offering a generalizable strategy for carbon-negative biomanufacturing.
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ACS Catalysis
·
2026
·
IF 13.6
Suiyang Dai,Jiahua Luo,Yuhan Zhou,Xin Liu,Yechao Su,Yabo Bian,Xueyan Sun,Ferenc Lónyi,Hongliang Li,Yongzhi Zhong,Jie Zeng
Ammonium bicarbonate (NH4HCO3) is a widely used nitrogen fertilizer that simultaneously offers nitrogen and carbon while consuming CO2 during its synthesis. Conventional NH4HCO3 production relies on the Haber−Bosch process to generate NH3 followed by CO2 neutralization, resulting in high pressure operating conditions (400−500 °C, 100−200 bar). Herein, we present a cascade plasma-thermal catalytic route that converts N2, H2O, and CO2 into NH4HCO3 under atmospheric pressure. In this process, non-thermal plasma activates N2 and H2O to generate NO and H2, bypassing thermodynamic constraints. The plasma-derived NO is then hydrogenated over Pt/HZSM-5 with supplementary H2 from water electrolysis to produce NH3. Finally, simultaneous CO2 absorption leads to the in situ formation of NH4HCO3, achieving a yield rate of 114.5 mmol h–1 at a discharge current of 0.4 A. This integrated approach offers a pathway for nitrogen fertilizer synthesis from air and water, representing a step toward carbon−nitrogen cycle coupling.
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Plasma Processes and Polymers
·
2026
·Vol. 23
·期 6
·e70198
·
IF 3.2
Kai Li,Jiajun Peng,Tianyu Liang,Feifan Zhang,Fangjie Zhou,Yuzhen Jin,Liancheng Zhang,Hua Pan,Fada Feng,Xuming Zhang
The reaction mechanism of plasma-catalytic CO 2 methanation remains unclear, especially regarding the Ni size effect. To address this, a tunable NiAl catalyst was explored. A linear correlation exists between methanation activity and Ni particle size: CO 2 conversion increases with larger Ni particles. The NiAl-300 catalyst (5.8 nm) achieved 86% CO 2 conversion and 100% CH 4 selectivity, while NiAl-500 (2.6 nm) reached only 63% and 98%, respectively. In situ DRIFTS revealed that larger Ni particles promote hydrogenation of formate and HCO species due to their efficient utilization of plasma-induced H radicals. This work provides theoretical support for rationally designing efficient catalysts in plasma-catalytic CO 2 methanation systems.
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Advanced Science
·
2026
·
IF 14.1
Dingran Wang,Bingyan Sun,Keran Wang,Di Fu,Ting Fan,Yanghui Lu,Tianfu Zhang,Kaige Wang
CO 2 hydrogenation to green methanol using renewable hydrogen offers a promising approach for achieving a sustainable carbon cycle. Among various catalyst designs, inverse catalysts have attracted growing interest due to their unique structural advantages. However, the performance of inverse catalysts, such as ZrO 2 /Cu, is hindered by their hydrophilic nature, while the systematic investigations into their surface wettability remain rare. In this study, we report a non-destructive hydrophobic modification strategy for ZrO 2 /Cu catalyst through physical mixing with polydivinylbenzene (PDVB). The optimized ZrO 2 /Cu-PDVB (1:1 mass ratio) catalyst achieves a methanol space-time yield of 920.10 mg CH3OH g cat − 1 h − 1 under mild conditions, outperforming the unmodified catalyst by 30%. Additionally, the optimized catalyst also demonstrates outstanding 200 h thermal stability. In situ DRIFTS and related analyses reveal that the PDVB effectively promotes water desorption and diffusion, alleviating its negative impact on the rate-determining step of formate hydrogenation. This also preserves the size, metallic state of Cu particles, and the abundance of oxygen vacancies, crucial for maintaining the active ZrO x -Cu interface. This work presents a simple, scalable method for adjusting the local microenvironment of inverse catalysts, highlighting the critical yet underexplored role of hydrophobic surface engineering in optimizing water-sensitive catalytic systems.
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PubMed
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AICHE JOURNAL
·
2026
·
IF 4.4
Yan Hou,Yue Zhang,Shaohui Tao,Lili Wang,Xiaoyan Sun,Shuguang Xiang,Li Xia,Guoxuan Li
Methyldiethanolamine (MDEA), an efficient and environmentally friendly absorbent, has been widely used in CO 2 capture. This study prepared and evaluated two novel ternary MDEA-based deep eutectic solvents (DES1 and DES2) for CO 2 capture performance. Experimental results show that the maximum CO 2 absorption capacities of DES1 and DES2 were 0.1237 and 0.1016 g CO 2 /g DES, with viscosities of 14 and 9.6 mPa s at 50 wt% water content. After five absorption–desorption cycles, DES1 maintained 82% of its initial absorption efficiency. Nuclear magnetic resonance analysis confirms the successful synthesis of DESs, which effectively absorb CO 2 . After regeneration, the structure remains unchanged despite chemical absorption, indicating the reversibility of MDEA-based DESs. Molecular-level analysis indicates that the DES1 capture CO 2 process involves physical absorption and chemical reactions. Specifically, ethanolamine reacts with CO 2 to form carbamate, and the interaction energy between CO 2 and MDEA is −2699.40 kJ/mol.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2026
·
IF 2.1
Minjie Gao,Congfei Zhu,Yasen Dai,Bingru Wang,Shuhang Ren,Weize Wu
Deep eutectic solvents (DESs) show great potential in the field of CO2 capture; however, the lack of systematic physicochemical property data remains a bottleneck constraining their rational design and industrial application. This study prepared six representative DESs and systematically characterized their key fundamental properties as absorbents: density, viscosity, thermal stability, and specific heat capacity. The results indicate that the chemical structure of the hydrogen bond acceptor has a decisive influence on the properties of the DESs. The viscosity and density of all DESs decreased significantly with increasing temperature. Thermogravimetric analysis revealed their varying thermal stabilities, with the onset decomposition temperature ranging from 366.52 K (menthol–ethylene glycol) to 415.17 K (choline chloride–ethylene glycol). The measurement of specific heat capacity data provides a key basis for evaluating solvent regeneration energy consumption. This study fills the gap in systematic property data of various DESs. Comprehensive analysis indicates that the choline chloride-ethylene glycol system achieves the best balance among viscosity, thermal stability, and specific heat capacity, making it a highly promising candidate based on its physicochemical property profile for CO2 capture among the studied systems. This work provides solid data support and theoretical guidance for the screening, design, and energy optimization of DESs in CO2 capture processes.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Jianyang Wei,Lirong Wang,Guanhua Liu,Luting Wang,Liya Zhou,Yunting Liu,Xiaobing Zheng,Yanjun Jiang
The main challenges in electroenzymatic CO2 reduction are the low solubility of CO2 and the high cost of the cofactor. Inspired by eukaryotic cell structures, this study designed a hollow zeolite imidazole framework (H-ZIF-8) with the dual functions of capturing CO2 and immobilizing dual enzymes. This platform was coupled with electrochemical cofactor (reduced nicotinamide adenine dinucleotide, NADH) regeneration for enzymatic CO2 reduction. The hollow structure of ZIF-8 retained the activity of formate dehydrogenase (FDH) and carbonic anhydrase (CA) in the obtained FDH&CA@H-ZIF-8, while achieving efficient CO2 reduction using substrate enrichment by CA and ZIF-8. 2-Hydroxy-1,4-naphthoquinone (HNQ) served as an electron mediator in the electrocatalytic step. The electroenzymatic system produced 3.12 mM formate within 3 h, which was 7.3 times that of the free enzyme system. Meanwhile, the immobilized enzyme retained 80.1% of the initial enzyme activity after 8 reuse cycles with high storage stability. This strategy provided an effective platform for addressing the limitations of CO2 solubility and cofactor regeneration in enzymatic CO2 conversion.
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JOURNAL OF SURFACTANTS AND DETERGENTS
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2026
·
IF 2
Di An,Le-Kai Hou,Chuan-Zong Fan,Jia-Chen Xing,Yi-Jie Jiang,Hua-Qiang Shi,Jia-Hui An,Wei Wang,Qun-Xing Luo
We synthesized a homologous series of alkyl amidines with chain lengths from C 4 to C 18 and systematically investigated their physicochemical properties, CO 2 responsiveness and applications. Key findings demonstrate a dual dependence of properties on the alkyl chain length and CO 2 -induced protonation. Both unprotonated and protonated surfactants show an inverted volcano-shaped relationship between surface tension and chain length, with optimal surface activity at intermediate lengths (C 8 –C 14 ), whereas oil–water interfacial tension shows minimal dependence on either chain length or CO 2 -induced protonation. Interestingly, these alkyl amidines exhibit distinct chain-length-dependent and CO 2 -switchable emulsification-demulsification behaviors. The unprotonated short-chain surfactants (C 4 –C 10 ) form O/W emulsions but cause demulsification upon protonation, whereas the unprotonated long-chain surfactants (C 12 –C 18 ) cannot emulsify but their protonated forms can stabilize O/W emulsions. The resultant emulsions stabilized by unprotonated short chains show a negatively charged interface due to hydrogen bond-induced water deprotonation by the amidine group, thereby generating the interfacial OH − ions. In contrast, emulsions stabilized by protonated long-chain amidines possess a positively charged interface via CO 2 -induced cationization. Importantly, the unique chain length dependence and CO 2 responsiveness were successfully leveraged for diverse applications, including clay stabilization, crude oil washing, and CO 2 -enhanced foam fire suppression. Graphical The structure-property-application relationships of CO 2 -responsive alkyl amidine surfactants was elucidated.
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ACS Catalysis
·
2026
·
IF 13.6
Hongxu Zhang,Mingyuan Liu,Wenjia Tian,Ke Liu,Mengyao Hao,Hairong Yu,Weikang Sun,Leilei Guo,Xiaoxu Tan,Kaiyu Gao,Tianyi Jiang,Chuanjuan Lü,Qianjin Kang,Cuiqing Ma,Longyang Dian,Ping Xu,Chao Gao
Enzymatic transformation is an attractive strategy for converting C1 compounds derived from CO2 into high-value products. However, its large-scale application is hampered by the necessity of costly cofactors such as ATP, NADH, and tetrahydrofolate. Here, we designed two costly cofactor-free enzymatic pathways that require only 5 enzymes and chemically synthesized cheap cofactor TPP for the production of platform compounds 3-hydroxypyruvate (3-HP) and pyruvate from formaldehyde. We screened and characterized two key enzymes, dihydroxyacetone oxidase catalyzing dihydroxyacetone oxidation and glyoxalase III catalyzing 3-hydroxypyruvaldehyde isomerization, in the designed pathways. We also engineered glyoxalase III SAV0551 toward stereoselectively isomerizing 3-hydroxypyruvaldehyde into l-glycerate to improve the production of 3-HP from formaldehyde. Then, we combined methanol oxidation with alcohol oxidase and the two designed pathways for enzymatic synthesis of 3-HP and pyruvate from CO2-derived methanol. The final concentrations of 3-HP and pyruvate reached 50.2 and 49.6 mM, with synthesis rates of 7.2 mmol C L–1 h–1 and 5.5 mmol C L–1 h–1, respectively. In addition, by coupling transketolase and pyruvate decarboxylase into the enzymatic system, we also achieved the biosynthesis of d-sedoheptulose-7-phosphate and acetoin from CO2-derived 3-HP and pyruvate with concentrations of 46.9 and 23.6 mM, respectively.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Kai Zhu,Zhenmao Zhang,Xinyin Bai,Fangfang Chang,Qing Zhang,Ge Li,Zhengyu Bai
Electrochemical pre-reconstruction creates CuO/Cu 2 O/Cu/CeO 2 @C heterointerfaces. • Carbon confinement stabilizes multivalent Cu interfaces during CO 2 electroreduction. • CeO 2 modulates the electronic structure and interfacial charge distribution of Cu. • Reconstructed interfaces tune the thermodynamics of *CO and *OCCO formation. • Ethanol Faradaic and cathodic energy efficiencies reach 75.6% and 30.9% at −0.9 V vs. RHE. The electrochemical CO 2 reduction reaction (CO 2 RR) to ethanol provides a carbon–neutral route for the sustainable production of value-added chemicals, yet achieving high ethanol selectivity remains challenging. Herein, we report a Ce-containing Cu-based oxide precursor embedded in a carbon framework, which undergoes electrochemical pre-reconstruction to form CuO/Cu 2 O/Cu/CeO 2 @C heterostructure featuring active multi-heterointerfaces. By optimizing the Ce content, the reconstructed catalyst delivers a high ethanol Faradaic efficiency of 75.6% and an energy efficiency of 30.9% at −0.9 V versus the reversible hydrogen electrode in a flow-cell reactor, outperforming most reported Cu-based CO 2 RR electrocatalysts. Comprehensive structural characterizations reveal that the carbon confinement layer mitigates excessive reduction of Cu species and stabilizes the multivalent Cu interfacial environment during CO 2 RR, while CeO 2 modulates the local electronic structure and induces interfacial charge redistribution over Cu sites. In situ characterization combined with theoretical calculations further reveals that interfacial environment modifies the relative thermodynamics of *CO and *OCCO formation. This work provides profound insights into interfacial charge-redistribution-mediated ethanol selectivity and provides a design strategy for high-performance advanced Cu-based CO 2 RR electrocatalysts. Download: Download high-res image (80KB) Download: Download full-size image
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