Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124587
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IF 7.5
Xiaoyan Han,Huiling Weng,Yani Shen,Jianjun Chen,Yu Xie,Qiulin Zhang,Ping Ning,Jiming Hao
CO 2 methanation is an important route for carbon emission mitigation and renewable energy storage. However, insufficient CO 2 activation and inefficient hydrogenation of surface intermediates at low temperatures remain major challenges. In this work, Ni/CeO 2 catalysts with distinct metal-support interaction degrees were constructed by regulating the interfacial contact of Ni-Ce, aiming to enhance the low-temperature methanation performance. The results suggest that Ni/CeO 2 with strengthened Ni-CeO 2 interfacial interaction exhibits more oxygen-vacancy-related defect sites, improved reducibility, and favorable Ni dispersion. These interrelated features collectively facilitate CO 2 adsorption/activation and intermediate conversion, thereby contributing to the enhanced low-temperature methanation performance. Specifically, the CO 2 conversion reached ∼80% at 250 °C. In situ Raman spectroscopy suggested the dynamic evolution of oxygen-vacancy-related defect sites during the reaction, while in situ DRIFTS suggested that CO 2 methanation may proceed through both the formate-mediated pathway and the CO* pathway. These findings suggest that tailoring the Ni-Ce interfacial interaction, together with the associated changes in oxygen vacancy related defects, reducibility, and Ni dispersion, may provide an effective approach to improving the low-temperature CO 2 methanation performance of Ni-based catalysts.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Jing Ma,Ziyan Yang,Yaxuan Du,Jun Wu,Jiali Li,Zhongfeng Geng,Zhaobang Zhang,Jing Zhu
The development of efficient and eco-friendly catalysts for the conversion of CO2 and propylene oxide (PO) to propylene carbonate (PC) is vital for carbon-neutral goals. To overcome the corrosion and environmental issues of halogenated ionic liquids (ILs), two novel halogen-free ILs were designed by pairing a p-toluenesulfonate anion with a carboxyl- or ether-functionalized 1-butyl-3-methylimidazolium cation. The carboxyl-functionalized IL, [HCPMIM][p-TSA], showed superior performance, achieving 98.60% PO conversion and 98.21% PC selectivity. Density functional theory (DFT) calculations confirmed its strong hydrogen-bond-donating ability, which led to the lowest energy barrier in the rate-determining step, consistent with the experimental data. This study provides a theoretical basis for designing efficient halogen-free catalysts and elucidates the reaction mechanisms.
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JOURNAL OF SOLUTION CHEMISTRY
·
2025
·Vol. 55
·期 3
·455-480
·
IF 1.3
Wang Yuting,Wang Min,Fu Xupeng,Wang Wenxue,Chai Liming,Wang Enna,Wei Xionghui,Wu Zhaojun,Zhang Jianbin
The impact of water on the physicochemical properties and CO 2 absorption capability of the N -methyldiethanolamine (MDEA) + polyethylene glycol 300 (PEG300) solution was explored. The molar ratio of PEG300 to MDEA was fixed at 0.3734: 0.6266, and the density and viscosity of the aqueous solutions were measured at P = 100.5 kPa and T = (298.15–318.15) K. Based on these measurements, the excess properties of the system were calculated. Meanwhile, spectral analysis confirmed the formation of intermolecular hydrogen bonds among MDEA, PEG300, and H₂O. Building on these findings, the influence of water content on the cyclic CO 2 absorption performance of the H₂O + (PEG300 + MDEA) system was systematically investigated, with particular emphasis on the regeneration behavior at 15 wt% MDEA concentration. Furthermore, the underlying mechanism of the cyclic CO₂ absorption process was elucidated using multiple analytical techniques. These insights provide certain theoretical support for the industrial application of PEG300 + MDEA aqueous systems in CO 2 capture.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Linfeng Fan,Ruyue Yin,Mingliang Wu,Yu Cui,Chunjin Ren,Chongyi Ling,Tang Tang,Jinlan Wang
An optimal oxygen spillover–SMSI window is theoretically identified to suppress catalyst deactivation. • Persistent Cu δ⁺ /Sb–O interfacial sites contribute to enhanced catalyst stability during CO 2 electroreduction. • Long-term electrolysis confirms that CuO x /Sb 2 O 4 maintains high FE CO for over 600 h at −0.9 V vs. RHE. Cu-based catalysts have shown great potential for CO 2 electroreduction, while facing a critical stability challenge. One fundamental cause lies in the fact that the active Cu δ ⁺ species are inherently prone to be reduced under operating conditions, leading to rapid structure reconstruction and activity degradation. Herein, a coupling strategy involving the deposition of CuO x on oxygen-donating metal oxide (CuO x /MO) was proposed to stabilize Cu δ+ via dynamic oxygen migration, thereby enhancing catalytic durability. A theoretical screening framework was developed, using oxygen vacancy formation energy ( E OV ) and CuO x desorption energy ( E CuOV ) as the descriptors to assess oxygen spillover propensity and metal-support interaction, respectively. This led to the selection of 9 promising candidates for stability enhancement, which were validated experimentally. Notably, Sb 2 O 4 stands out as the optimal support, endowing CuO x exceptional long-term stability, maintaining a CO Faradaic efficiency of 91.2% at –0.9 V vs. RHE for over 600 h of continuous operation. Comprehensive characterizations further revealed that sustained lattice-oxygen-mediated interfacial oxygen exchange, together with strong metal-support interactions, is proposed to contribute to the robust Cu δ+ /Sb-O interface, promoting CO desorption and suppresing reconstruction. This work elucidates the dynamic evolution of CuO x /MO interfaces under CO 2 RR conditions and establishes a generalizable design paradigm for stabilizing reactive oxidation states via engineered oxygen spillover. Download: Download high-res image (184KB) Download: Download full-size image A lattice-oxygen-overflow strategy is proposed to stabilize Cu δ⁺ sites for durable CO 2 electroreduction to CO. DFT screening identifies Sb 2 O 4 as an optimal oxygen-donating support with suitable oxygen vacancy formation energy and strong CuO x –support interaction. Dynamic oxygen migration from Sb 2 O 4 preserves the Cu δ⁺ /Sb–O interface, suppresses Cu reconstruction, and promotes CO desorption. As a result, CuO x /Sb 2 O 4 achieves 91.2% CO Faradaic efficiency at –0.9 V vs. RHE and maintains stable operation for over 600 h.demonstrating a general design principle for stabilizing reactive oxidation states through engineered lattice oxygen spillover.
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Energy Technology
·
2026
·Vol. 14
·期 8
·e70614
·
IF 3.6
Bing Zhang,Yu Zhang,Zhengxin Lu,Song Zhou,Ping Li,Kui Xu,Yonghua Chen
Electrocatalytic CO 2 reduction reaction (CO 2 RR) stands as a pivotal strategy for the selective conversion of CO 2 into high-energy-density hydrocarbons, offering a promising avenue for carbon neutrality. Cu-based electrodes have emerged as a highly potential platform for the production of diverse products, yet their practical application is hindered by the crystallization regulation of electrocatalysts achieving high selectivity for multielectron products. Here, we report Cu-based electrodes, deposited on carbon paper via facile one-step coelectrodeposition methods, for efficient electrocatalytic CO 2 RR. The introduction of trace Ni was found to smooth the surface of Cu-based electrocatalysts, thereby facilitating the electron transfer at the catalytic interface. For CuNi 0.3% electrode, a maximum Faraday efficiency of 30.5% and a CH 4 yield rate of 16.4 mg h −1 cm −1 were achieved at −1.4 V versus RHE, outperforming the Cu electrode (17.9% FE) and the CuNi 0.6% electrode (26.9%). This enhancement might be attributed to the superior surface of the CuNi 0.3% electrocatalyst, with the trace amount of Ni 2+ codeposition playing a critical role in optimizing the smooth surface of the Cu electrode. Density functional theory calculations further revealed that Ni addition is thermodynamically favorable for the deep hydrogenation of *CO by lowering the formation energies of *CO and *COH intermediates.
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Molecular Catalysis
·
2026
·
IF 4.3
Song Wu,Xiangqian Guo,Chenhui Qiu,Jinfeng Zhang,Hui Wan,Guofeng Guan
Light-driven CO 2 conversion to high-value chemicals has emerged as promising but challenging strategy to alleviate global energy and environmental concerns. The efficacy of this process hinges critically on the design of advanced catalysts. Herein, the metallic co-catalysts Pt deliberately anchored onto the surface of La 0.8 Sr 0.2 Co 0.7 Fe 0.3 O 3 (LSCFO) nanotubes was constructed via direct coaxial electrospinning method. Experimental analyses and density functional theory (DFT) simulations confirmed that the incorporation of Pt creates additional active sites and suppresses the recombination of photo-generated electron-hole pairs, thereby enhancing photocatalytic CO 2 reduction capability. Under visible light illumination, the optimized Pt 6 /LSCFO catalyst demonstrated a remarkable CH 3 OH yield of 7.20 μmol·g⁻¹·h⁻¹, outperforming pristine LaCoO 3 by a factor of 3.48. Moreover, the catalyst retains its structural integrity and catalytic performance over four consecutive cycles, demonstrating excellent stability. This work presents an integrated strategy via one-step coaxial electrospinning method for constructing high-performance composite photocatalysts.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 2
·121896
·
IF 7.5
Zhongliang Sun,Shuonan Cao,Mengru Xin,Shoukai Guo,Yu Zhang,Qiang Wang,Liqin Sun
Microalgae are efficient biological platforms for CO 2 capture and renewable bioresource production; however, carbon assimilation efficiency remains a major bottleneck. In this study, symbiotic bacteria capable of secreting extracellular carbonic anhydrase (CA) were isolated from natural algal-associated environments to enhance CO 2 hydration and utilization in Chlorella sorokiniana . Among six CA-secreting isolates, three strains exhibited high extracellular CA activities and promoted algal growth without inhibitory effects. Co-cultivation with Bacillus safensis YD-1 and B. licheniformis YD-6 increased biomass productivity by up to 74 % and lipid content by 65–70 % compared with axenic controls, while mitigating total inorganic carbon (TIC) depletion during late-stage cultivation. The co-culture systems maintained extracellular CA activities of 3.6–4.8 U/mL and reduced TIC loss to 8.9–16.0 %, compared with 20.3–30.5 % in controls. Immobilization of YD-1 cells using alginate–calcium beads enabled repeated reuse over three cultivation cycles, retaining > 80 % of CA activity and sustaining consistent growth enhancement. These results demonstrate that immobilized CA-secreting symbiotic bacteria provide a self-regenerating and reusable biological strategy to alleviate carbon limitation, offering a practical and scalable approach for improving CO 2 utilization and biomass production in microalgal cultivation systems.
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Journal of Energy Chemistry
·
2026
·
IF 15.6
Feifei Yang,Tianyu Zhang,Shijian Lu
Single-atom catalysts (SACs) with a two-dimensional (2D) material as the support offer peculiar active sites at edges and in planes, which differ significantly in their chemical environments and consequently in their catalytic performances in reactions. Herein, we report that Pt single atoms anchored at the edges of 2D MoS 2 nanosheets deliver dramatically high activity for CO 2 hydrogenation to CO, in contrast to Pt single atoms as well as their aggregations of 2D-rafts on the in-plane MoS 2 showing inferior activity. By a combination of experimental and theoretical studies, it was found that the activation of CO 2 was significantly facilitated on the Pt single atoms with the synergetic effect of its neighboring Mo at the edges, which readily dissociates into gaseous CO with a low energy barrier. Pt, which is isolated by the S-coordinated surroundings on the in-planes, is inert toward CO 2 adsorption and activation, thus leading to poor activity. This research reveals the close association between the catalytic performance of SACs with their chemical environments, and provides insights into the mechanism modulated by the synergetic effect between single-atom active sites and the support.
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APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Yifu Wang,Junwu Mou,Biao Gao,Chaianansutcharit Soamwadee,Kuchonthara Prapan,Limin Guo
The hydrogenation of CO 2 to methanol is a promising strategy for renewable carbon utilization, where indium oxide loaded zirconia catalysts have been extensively studied. However, the influence of monoclinic zirconia (m-ZrO 2 ) support size on the structure-activity relationship remains insufficiently understood. Here, we systematically investigate the size effect of m-ZrO 2 supports on the structure, surface chemistry, and catalytic performance of In 2 O 3 /m-ZrO 2 catalysts. Comprehensive characterizations reveal that an optimal ZrO 2 grain size (∼13 nm) is associated with strengthened In 2 O 3 -ZrO 2 interaction and an increased concentration of thermally induced oxygen vacancies. In-situ DRIFTS confirms a formate-mediated pathway and enhanced formate intermediates conversion. Consequently, 5 %In/Zr-600 exhibits the highest methanol yield (0.43 g MeOH g cat −1 h −1 ). In comparison, smaller supports suppress methanol selectivity due to weak interfacial interaction, while larger supports promote In 2 O 3 crystallization and cause surface area loss, limiting activity and stability. These findings provide insight into how support grain size influences metal oxide and support interactions and catalytic behavior within the In 2 O 3 /m-ZrO 2 system.
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ACS Applied Materials & Interfaces
·
2026
·
IF 8.2
Tianlong Tan,Hai Liu,Wenlong Cao,Lei Yang,Shujing Ju,Caiyu Chen,Ewald Janssens,Guowei Han,Dachun Lu,Jue Wang,Qinfang Zhang
The electrochemical CO2 reduction reaction (CO2RR) is one of the most promising pathways to achieving carbon neutrality. However, in acidic electrolytes, the CO2RR tends to suffer from competitive hydrogen evolution side reactions. Alkaline electrolytes are typically employed to suppress side reactions and promote the formation of valuable multicarbon (C2+) products (e.g., ethylene(C2H4)). In this study, we fabricated surface-loaded copper cluster catalysts with particle sizes below 5 nm by magnetron sputtering and inert gas condensation in combination with cluster beam deposition. This approach enabled precise control over the catalyst surface structure, allowing for in-depth investigation of the synergistic effects between the catalyst microstructure and its catalytic microenvironment. We demonstrate that the Faradaic efficiency (FE) for CO2-to-C2H4 conversion exceeds 50% across a broad current density range of 50 to 180 mA cm–2 in a flow cell using 1 M KOH electrolyte. Compared with a pristine Cu/PTFE catalyst, the optimized Cu cluster catalyst not only exhibits a significant enhancement in FEC2H4 but also expands the effective current density range. Furthermore, finite element simulations combined with in situ Raman spectroscopy reveal synergistic interactions among interfacial species (e.g., *CO, OH–, and K+). Therefore, this study proposes a general strategy to regulate the dynamic evolution of catalytic interfaces through an initial nanostructure design, thereby opening a promising avenue for the selective conversion of CO2 to ethylene.
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PubMed
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ACS Omega
·
2026
·
IF 5.2
Malesela A. Mafokoane,Peixi Liu,Xiaoxia Ou,Nicholas M. Musyoka,Fei Chang
The reduction of carbon dioxide (CO2) to methanol (CH3OH), is presently constrained by energy-intensive processes requiring high temperatures and pressures to overcome kinetic and thermodynamic limitations. This work unveils for the first time a reaction pathway for alkali and alkaline earth metal hydrides (LiH, NaH, KH, MgH2, CaH2, and BaH2), enabling the activation and selective reduction of CO2 to methanol under ambient pressure. This finding represents a significant departure from the established paradigm, which exclusively produced methane at moderate pressures (0.1–1 MPa). Temperature-programmed reaction studies reveal that these metal hydrides function synergistically as both hydrogen sources and promoters for CO2 reduction, exhibiting hydrocarbon production within specific temperature windows. Systematic screening identifies lithium hydride (LiH) as the most effective material, with a maximum production rate of 0.182 μmolMeOH·molmetal–1·h–1 at 245 °C under ambient pressure, highlighting a structure–activity relationship governed by metal-formate stability. Through mechanistic investigation, we elucidate a formate (HCOO*)-mediated pathway wherein the hydride ion serves as a potent nucleophile, directly reducing CO2 without the need for high H2 partial pressures. This discovery provides a transformative framework for the sustainable synthesis of CH3OH and lays the groundwork for the development of next-generation materials incorporating reactive ionic hydrides for the conversion of CO2 under mild conditions.
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PubMed
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ENERGY & FUELS
·
2026
·
IF 5.3
Jian Wen,Yangfeng Zheng,Cheng Zhai,Hexiang Xu,Yu Wang,Hongda Wen,Zijian Yu,Huijun Xing
Injecting CO2 foam fracturing fluid into coal seams leads to modifications in the coal’s pore structure, which directly affects coalbed methane (CBM) recovery. Among the influencing factors, the duration for which the CO2 foam remains within the coal seam plays a critical role. This study examines how the pore structure of Zhangminggou bituminous coal evolves after treatment with a CO2 foam fracturing fluid for different durations. Experiments were conducted at 40 °C and 5 MPa, with treatment durations of 3, 6, 12, 24, and 48 h. The evolution of the pore structure in modified coal was analyzed through nuclear magnetic resonance and low-temperature nitrogen adsorption techniques. Results show that pore structure evolution is strongly time-dependent. Relative to untreated coal, foam-treated coal exhibits an increase in micropores but a decrease in average pore size, alongside a moderate rise in mesopores and a marked increase in macropores and fractures. Fractal analysis of NMR images indicates that the opening size of the generalized fractal dimension spectrum and the width of the multifractal singularity spectrum both increase with treatment time, which reflects growing spatial complexity and heterogeneity in pore distribution. Low-temperature nitrogen adsorption results reveal that the specific surface area, total pore volume, and average pore diameter increase with treatment time, following a power-law relationship. The pore volume distribution shifts from 2–10 nm toward >50 nm, with a rising proportion of pores larger than 50 nm. These findings provide valuable insights for optimizing the CO2 foam fracturing parameters in practical applications and enhancing CBM recovery.
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