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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POLYMER
·
2026
·
IF 5.1
Xu Jiang,Wenwen Jiang,Xinqi Xie,Xinyi Shen,Yu Tang,Chen Wang,Huanwang Jing,Faliang Gou
Three monoimidazole-modified cobaltoporphyrins with different substitution positions were designed and synthesized as bifunctional homogeneous catalysts for the alternating copolymerization of propylene oxide (PO) and CO 2 to produce biodegradable poly(propylene carbonate) (PPC) under mild conditions without a cocatalyst. Their catalytic performance strongly depends on the ligand skeleton, which determines product selectivity. Under optimal conditions, catalyst X- o 4 showed high PO conversion, polymerization selectivity, high molecular weight polycarbonate, and narrow molecular weight distribution. Kinetic studies using X- o 4 and bisimidazole-modified J- o 4 gave apparent activation energies for polycarbonate and cyclic carbonate. Based on structural and experimental data, a competition mechanism between polymerization and cycloaddition is proposed. Density functional theory (DFT) calculations support this mechanism, explaining the temperature-dependent selectivity and the different behaviors of mono- and bis-imidazole catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Huilin Li,Xuechong Ding,Teng Zhou
Reducing regeneration energy remains a central challenge in post-combustion CO 2 capture by chemical absorption. In this work, nine aqueous MDEA/DMEA/PZ blends were systematically screened using thermodynamic performance indicators, including the heat of absorption, heat capacity, and equilibrium CO 2 absorption capacity. Two formulations, D30P10 (30% DMEA +10% PZ) and M5D25P10 (5% MDEA +25% DMEA +10% PZ), were identified as the most promising candidates for achieving low regeneration energy. These two solvents were further evaluated against two benchmarks, 30 wt% MEA and M30P10 (30% MDEA +10% PZ), in cyclic absorption–desorption experiments. Among them, M5D25P10 delivered the best overall balance of stable cyclic performance and a cyclic capacity about 0.55 mol CO 2 /mol amine. Benefiting from its high cyclic capacity and low heat of absorption, this solvent achieved a regeneration energy of 2.98 GJ/t CO 2 , which was 21.2% and 4.5% lower than those of 30 wt% MEA and M30P10, respectively. Kinetic performance indicators, including the initial absorption rate ( r abs ini ) and the overall mass transfer coefficient ( K G ), were also evaluated, and M5D25P10 exhibited the highest mass transfer coefficient among all tested solvents. These results collectively confirm that M5D25P10 is a highly promising solvent for post-combustion CO 2 capture. Moreover, a robust empirical correlation between r abs ini and K G was established for the first time, providing a rapid and solvent-efficient means of estimating mass-transfer performance.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123805
·
IF 7.5
Jianxin Zhang,Liu Yang,Hongwei Yang,Zhenhuan Li,Shanghan Han,Xiaoyao Tan
In gas separation processes, magnetic induction heating (MIH) offers a promising alternative to conventional heating by avoiding its poor energy efficiency. In this paper, we report a CO 2 sorbent comprised of magnetic nanoparticles (MNPs), hollow fiber, and solid amine for efficient direct air capture (DAC) of CO 2 . The MNPs have the nature of temperature controlling, which making the composite hollow fibers have self-regulating temperature properties. Furthermore, the maximum temperature of composite hollow fiber can be tuned by varying the MNPs content. The heating rate and cooling rate of the composite hollow fibers were compared with those of conventional heating method. The results showed that the magnetic nanoparticles composited hollow fibers exhibited higher heating rate and cooling rate. For the self-regulating temperature solid amine hollow fibers, the magnetic nanoparticle content has effects on CO 2 adsorption capacity, desorption rate and cooling rate. Increasing the magnetic nanoparticles content led to a trade-off effect between heating rate and CO 2 adsorption capacity. The CO 2 adsorption capacity decreased whereas the heating rate increased. The advantage of induction heating over conventional heating for regenerating the CO 2 sorbent were demonstrated. Specifically, the PEI-ECH-MNP20%-PAN HFs achieved heating rate, cooling rate, and desorption rates of 6.7 ℃ min −1 , 3.8 ℃ min −1 , and 0.11 mmol CO 2 g −1 min −1 , respectively. The induction heating method yielded a higher heating rate, cooling rate and desorption rate than conventional heating, which is expected to significantly shorten the cycle time, and thus improve the overall efficiency of the CO 2 capture system. For direct air capture, PEI-ECH-MNP20%-PAN HFs exhibit a CO 2 adsorption capacity of 2.59 mmol g −1 , and saturated PEI-ECH-MNP20%-PAN HFs can be efficiently regenerated via a magnetic induction heating-vacuum swing (MIH-VS) desorption process.
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AICHE JOURNAL
·
2026
·
IF 4.4
Yirong Wang,Qin Sun,Junbo Li,Tiantian Liu,Xiaohua Li,Liangzhi Yu,Sen Wang,Prasert Reubroycharoen,Lizhi Wu,Yu Tang,Li Tan
Propylene is a key chemical. Propane dehydrogenation (PDH) over non-noble cobalt catalysts suffers rapid deactivation from sintering and coking. Herein, we report a core–shell catalyst (1.0Co/BEA@ x Si) with a mesoporous silica shell on Co-impregnated dealuminated Beta zeolite. The silica shell enhances Co dispersion and modulates Co reduction: it promotes the formation of active tetrahedral Co 2+ sites from Co 3 O 4 while suppressing over-reduction to metallic Co 0 . The optimized 1.0Co/BEA@1.0Si maintains ~99% propylene selectivity and achieves a formation rate of 71.0 gC 3 H 6 ·g Co −1 ·h −1 after 980 min, far surpassing uncoated 1.0Co/BEA and most reported Co-based PDH catalysts. In situ and post-reaction analyses show the shell strengthens propane adsorption/activation and reduces coke formation. Core–shell engineering thus stabilizes active metal states via local redox microenvironment modulation, offering new design principles for robust alkane dehydrogenation catalysts.
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Science Advances
·
2026
·Vol. 12
·期 35
·
IF 13.9
Lei Li,Ming Zheng,Chunhua Cui
The origin of abiotic methane in Earth’s shallow crust remains unresolved, as existing theories require extreme conditions or catalytic surfaces. Here we show that hydrogen bond reorganization in pressurized bicarbonate aqueous solution (3 MPa, 25°C) activates radical chemistry for CO 2 -to-methane conversion (0.6 μM for 14 days). Through electron paramagnetic resonance (EPR) and in situ Raman spectroscopy, we demonstrate that pressure-induced restructuring of water’s hydrogen bond (HB) network generates hydrated electrons (e − aq ) and hydrogen radicals ( • H), which drive CO 2 reduction via a solution-chemistry mechanism independent of mineral catalysts. This water-mediated radical process provides experimental evidence for abiotic methanogenesis under geologically relevant conditions, fundamentally redefining water’s role from solvent to redox-active participant in subsurface carbon cycling. The findings open alternative avenues for understanding natural hydrocarbon reservoirs and engineered carbon sequestration.
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PubMed
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
·
2026
·
IF 2.2
Kaili Liao,Bowen Wu,Minglu Shao,Haiqun Chen,Lipei Fu,Ailian Chang,Daigang Wang,Lifeng Chen,Yingrui Bai,Xingtao Wang,Bing Feng,Zhiguo Yang
Emulsification flooding is a key mechanism for enhanced oil recovery. However, while strong emulsification significantly improves displacement efficiency, it concurrently poses substantial challenges to the subsequent oil–water separation of produced fluids. Therefore, developing smart surfactants that integrate robust emulsifying capacity with facile and efficient demulsification functionality is of considerable importance. In this study, a novel CO2-responsive surfactant (DFD-DA) featuring a dynamic imine bond was synthesized via a Schiff base reaction between disodium 4-formylbenzene-1,3-disulfonate (DFD) and dodecylamine. Its interfacial activity, emulsification performance, and oil displacement efficiency were systematically evaluated. The CO2-responsive demulsification behavior was examined, and the underlying emulsification mechanism was further elucidated through molecular dynamics simulations, complemented by experimental evidence. Results demonstrate that blending DFD-DA with lauroamidopropyl hydroxysulfobetaine (LHSB) at a 1:2 molar ratio significantly reduces interfacial tension to an order of 10−1 mN/m. This blended system exhibits exceptional emulsification performance, achieving an emulsified oil rate (E0) of 91.67% ± 1.05% and an emulsification index (EI) of 1.48 ± 0.03, along with remarkable CO2 responsiveness. Microscopic oil displacement experiments confirmed that the system effectively mobilizes crude oil and enhances the recovery of residual oil. Molecular simulation results provided supplementary insights into the emulsification process and the stabilization mechanism at the molecular level. This work presents a promising CO2-responsive surfactant system for both enhanced oil recovery and controllable demulsification in high water-cut oilfields.
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AICHE JOURNAL
·
2026
·
IF 4.4
Peixin Zhang,Chaoming Hu,Zhenglong Zhu,Zhenwei Zhou,Hao Wang,Jingwen Chen,Shixia Chen,Zhenyu Zhou,Shuguang Deng,Jun Wang
The practical application of metal–organic frameworks (MOFs) for CO 2 capture requires balancing high efficiency, cyclability, and scalable production. Herein, we report a novel MOF adsorbent, Cu 3 (ntrz) 2 (ox) 2 , which allows for low-cost and scalable synthesis in aqueous solutions under ambient conditions. Its tailored large pocket-like cavities interconnected by narrow pore apertures provide exceptional CO 2 adsorption capacities of 6.80 and 3.48 mmol g −1 at 1.0 bar and 0.15 bar (298 K), achieving a record-high VPSA working capacity of 5.03 mmol g −1 within 0.05–1.0 bar. Shaped pellets retain 95% CO 2 adsorption capacity and good mechanical strength, fulfilling industrial requirements. Experimental VPSA analysis demonstrates that a 15% CO 2 gas-stream can be enriched to 91.37% and 95.06% with productivities of 0.402 and 1.86 m 3 t −1 h −1 within 0.08–1.0 bar and 0.08–6.0 bar, outperforming zeolite 13X. The adsorption behaviors and mechanisms are elucidated via Grand Canonical Monte Carlo and dispersion-corrected density functional theory simulations.
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Journal of Materials Chemistry A
·
2026
·
IF 9.2
Yangyang Zhao,Yijian Wang,Xiaoyu Wang,Xingchen Feng,Tao Cong,Juntao Feng,Pei Wang,Kai Yang,Xifeng Ding
Solid oxide electrolysis cells (SOECs) offer a promising route for electrochemical CO 2 conversation to sustainable fuels, but their widespread adoption is hindered by the lack of cathodes combining high catalytic activity and stability. To address this challenge, we developed an in-situ interface-engineered La 0.6 Sr 0.4 Fe 0.95 Ti 0.2 O 3-δ cathode (R-LSF 0.95 T) cathode featuring exsolves Fe nanoparticles. The optimized R-LSF 0.95 T-based cell delivers a current density of 780 mA cm -2 at 1.5 V and 800 °C in pure CO 2 atmosphere, representing a 23.2% improvement over mechanically mixed electrode. This performance enhancement arises from synergistic metal-oxide hetero-interfaces, where the reduced perovskite substrate promotes CO 2 adsorption and oxygen-ion transport, while the Fe nanoparticles provide abundant active sites and reduce activation barrier for CO 2 reduction. Notably, the Fe-decorated perovskite demonstrates superior carbon deposition compared to Ni-based cathodes owing to its moderate activity. Consequently, the electrolysis cell maintains exceptional stability over 100 h at 1.5V and 800 ℃, with interfacial robustness further enhanced through redox cycling due to reinforced anchoring effect with more minute Nano-Fe exsolution. This work establishes a novel materials design paradigm that reconciles the activity-stability trade-off in SOEC cathodes through the combination of moderately active catalysts with interface reinforcement, offering new pathways for developing durable, high-performance CO 2 electrolysis systems.
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Plasma Processes and Polymers
·
2026
·Vol. 23
·期 5
·e70179
·
IF 3.2
Liangping Xiao,Rui Zhang,Tianyu Li,Jiahui He,Yu Liang,Xiubin Luo,Fuxue Wang,Xiao Liu,Jiannian Yao,Rusen Zhou
Two-dimensional (2D) materials have demonstrated excellent application prospects in electrocatalysis due to their unique anisotropy, high densities of exposed atoms, and tunable surface chemistry. However, the top-down exfoliation of few-layer nanosheets by breaking van der Waals interactions often introduces external intercalating molecules or solvent molecules, which adversely affect their performance in electrocatalytic reactions. Herein, we report a liquid-phase plasma bubbles treatment method for the exfoliation and preparation of few-layer Bi 2 Se 3 nanosheets. As no external intercalating molecules are introduced, and the as-exfoliated few-layer nanosheets possess a higher density of unsaturated bonds, they exhibit outstanding performance in the electrocatalytic carbon dioxide reduction reaction (CO 2 RR). The Faradaic efficiency for CO 2 electroreduction to formate exceeds 90%, with catalytic stability maintained for up to 100 h. Furthermore, this exfoliation method demonstrates broad applicability, successfully producing few-layer MoS 2 , WS 2 , and WSe 2 nanosheets. This work provides a new strategy for the synthesis of high-performance few-layer nanosheets for electrocatalysis.
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