Nature Communications
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2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Wang Ruonan,Zhang Mingjia,Liu Jingjing,Wu Xu,Zhang Shule,Zhong Qin,Yao Jianfeng
Scaling up methanol yields by artificial photosynthesis at a modest cost remains thermodynamically challenge. Designing concerted reaction sites to control intermediate evolution and stimulate proton-coupled electron transfer (PCET) is necessary. Here we show a nickel-titanium-based catalyst that achieves near-millimolar hourly methanol yields with 99.79% selectivity and a solar-to-chemical conversion efficiency of 2.23%. This catalyst is synthesized through one-step etching of NiTi-layered double hydroxide, which generates abundant unsaturated sites, along with the in-situ formation of amorphous TiO 2 . Revealed by in-situ characterizations, these defect-rich units effectively suppress the formation of undesirable carbonate while promoting the favorable *COOH intermediate. Furthermore, theoretical simulations confirm this *COOH boost facilitates the production of *CO and accelerates the PCET steps. This work significantly advances efficient methanol production by artificial photosynthesis and offers fundamental insights into controlling reaction pathways for renewable fuel synthesis.
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JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Weihao Liu,Xu Jiang,Yan Yang,Lei Guo,Haoyang Wang,Lu Shao
Constructing high-performance mixed matrix membranes (MMMs) with highly permeable polymers of intrinsic microporosity (PIMs) and metal-organic frameworks (MOFs) faces critical challenge of poor interfacial compatibility between MOF fillers and the polymer matrix and difficulty in maintaining a defect-free interface at high filler loading (over 30 %). In this study, a Bi-HHTP loading as high as 50 wt% and uniform dispersion with excellent interfacial integrity is achieved in our high-performance MMMs through the elaborate design of multiple synergistic interfacial interactions, including hydrogen bonding between the phenolic hydroxyl groups of the 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) ligand in the Bi-HHTP filler and the cyano groups in the PIM-1 matrix and π-π stacking between their benzene ring structures. The optimized MMM exhibits a remarkable CO 2 permeability up to 4021 Barrer with an ideal CO 2 /N 2 selectivity of 42.1 which substantially outperforms the neat PIM-1 membrane and exceeds the 2019 upper bound. The enhanced separation performance of the MMMs stems mainly from the significant increase in CO 2 solubility selectivity with Bi-HHTP loading, which benefits from the inherent CO 2 affinity of Bi-HHTP and the effective suppression of N 2 dissolution by the rigidification of PIM-1 chain segments induced by strong interfacial interactions. Most importantly, the resulted high-loading MMMs exhibited remarkable structural stability, showing strong resistance to both physical aging and CO 2 -induced plasticization. This strategy overcomes the loading bottlenecks of state-of-the-art MMMs and contributes advanced membrane materials for efficient CO 2 capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Mian Zhu,Chao Lyu,Feng Dai,Jingxian Liu
To develop an environmentally friendly CO 2 capture technology, composite adsorbent beads were synthesized through the in situ growth of ZIF-8 in a nanocellulose gel scaffold prepared from pine needles-derived cellulose. The composite beads were subsequently functionalized with three ionic liquids ([BMIM][PF 6 ], [BMIM][BF 4 ], and [EMIM][TF 2 N]), which induced partial dissolution of the nanocellulose. This process resulted in the formation of unique wrinkled microstructures, resembling rice grains in morphology but exhibiting higher compressive strength. Notably, the IL-loaded CNF/ILs@ZIF-8 composites exhibited significantly superior adsorption performance over unmodified CNF@ZIF-8 (CZ) beads. Under static conditions (3 bar, 273 K), all three functionalized CNF/ILs@ZIF-8 variants enhanced CO 2 uptake capacities by > 46 %, with the [BMIM][PF 6 ] modified beads retaining 85.36 % of initial adsorption capacity after six adsorption–desorption cycles. Furthermore, under competitive dynamic adsorption (1 bar, 273 K), the [BMIM][BF 4 ] modified beads achieved a 43.12 % enhancement in CO 2 /N 2 selectivity compared to CZ. This work provides a MOF granulation strategy with process safety and environmental sustainability, potentially extending MOF applications in gas adsorption technologies.
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THERMOCHIMICA ACTA
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2025
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IF 3.5
Wenke Zhang,Jianzhong Liu,Haiou Wang,Xueqin Liao,Jianren Fan
Aluminum (Al) combustion in CO 2 was investigated to assess carbon sequestration potential. Theoretical and experimental results identified C(s), Al 4 C 3 (s), and CO(g) as primary products, with C(s) formation being most thermodynamically favorable. Al oxidation in CO 2 proceeded through three stages, with the second stage (activation energy: 260–268 kJ·mol⁻¹) exhibiting the highest reactivity. Kinetic analysis indicated an Anti-Jander/D1 mechanism for this dominant stage. Reducing particle size from 25 μm to 0.1 μm at 0.1 MPa shortened ignition delay by 664 ms and increased combustion temperature by 847 K. Characterization confirmed carbon incorporation in products (Al 2 O 3 /Al 4 C 3 ) and demonstrated enhanced combustion efficiency and carbon fixation with smaller particles or higher pressures. These findings provide critical insights for Martian in-situ resource utilization and carbon capture technologies.
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Energies
·
2025
·Vol. 18
·期 16
·4237
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IF 3.2
Xinmei Wang,Junqiang Han,Jianing Ni,Changlei Qin
With the advancement of global carbon reduction efforts and the rapid development of battery industries, the scale of spent lithium-ion batteries (LIBs) has increased dramatically. Extracting lithium from spent LIBs to synthesize Li4SiO4sorbents not only addresses the challenge of battery recycling but also reduces the production cost of CO2sorbents, making it a research hotspot. However, the CO2adsorption behavior of these sorbents under the effect of impurities may differ from the traditional Li4SiO4, and there is a lack of systematic research on the adsorption kinetics. To address this issue, two Li4SiO4sorbents are prepared from spent ternary LIBs, and their adsorption kinetics are comprehensively investigated using classical kinetic models. Results show that the reaction order of LSO and Na-LSO is 0.41 and 1.63, respectively, with activation energies of 72.93 kJ/mol and 99.23 kJ/mol in the initial kinetic-controlled stage, and 323.15 kJ/mol and 176.79 kJ/mol in the following diffusion-controlled stage. In the cyclic processes, loss-in-capacity is observed on LSO due to the simultaneous decrease in rate constants in both the kinetic and diffusion-controlled stages, while Na-LSO could almost maintain its capacity by having a much bigger rate constant during the kinetic-controlled stage. This study reveals the adsorption kinetics of Li4SiO4prepared from spent LIBs and could provide theoretical support for the targeted design of efficient and low-cost CO2sorbents.
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Science Advances
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2025
·Vol. 11
·期 12
·
IF 12.5
Xiaoran Zhang,Yanhong Lyu,Jingjing Ding,Xin Wang,Bernt Johannessen,San Ping Jiang,Jianyun Zheng
l-phenylalanine (l-Phe), an essential amino acid for humans, is widely used as building blocks. Currently, l-Phe is obtained via biosynthetic methods including microbial and enzymatic processes, but their tightly complex feedback regulation and lengthy reaction steps lead to a low practical yield of l-Phe. Here, we have designed a hierarchical Si-based photocathode for l-Phe synthesis by photoelectrochemical coupling of waste CO2 and nitrophenyl ethane, achieving a high yield rate of 37.5 μg·hour−1·cm−2 and a remarkable Faradaic efficiency of 21.2% at low applied potential under 1 sun illumination. The hierarchical structure with CuO-TiO2-C mixtures dispersed in amorphous TiO2 layer/n+p-Si creates an internal built-in electric field and forms plentiful conducting channels to efficiently realize the injection of electrons into Cu and Ti sites. These Cu and Ti sites adsorb and activate the CO2 and nitrophenyl ethane, respectively, cooperatively facilitating the l-Phe synthesis. This work introduces an environmentally friendly and highly efficient approach for converting solar energy into valuable amino acid products.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2025
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IF 4.6
Fan Yang,Siqing Liu,Mengdie Yang,Deting Fei,Yunxin Zhang,Panjie Li,Xiaojun Luo,Qiwei Wang
The development of innovative materials capable of detecting heavy metal ions is a crucial goal in the field of environmental remediation. However, achieving high selectivity for specific metal ions remains a challenge. This study designs a novel imine-based COF via Schiff base condensation for efficient detection of cobalt ions (Co 2+ ) in environmental samples. The π-conjugation system provides excellent fluorescence properties. The COF contains tertiary amine and imine structures with nitrogen and oxygen atoms, enabling coordination with Co 2+ as a Lewis base. This interaction disrupts the conjugated structure, causing fluorescence quenching. The experimental results demonstrate that our proposed method stands out in Co 2+ detection, distinguished by its remarkable simplicity, exceptional sensitivity, rapid response time, and easy operability. The novel imine-based COF sensor exhibits high sensitivity (limit of detection = 8.5 × 10 −13 M), excellent selectivity and stability in fluorescence detection, enabling accurate identification of Co 2+ in complex environments. This research not only presents an efficient and practical approach for the detection of Co 2+ but also offers novel theoretical perspectives on the design and application of imine-based COF. The findings lay a solid foundation for the development of COF-based environmental monitoring technologies.
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ACS Catalysis
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2025
·
IF 13.1
Zhiwei Liang,Shan Tang,Siyu Chen,Lanqi Ning,Jijie Wang,Can Li
Zinc–zirconium oxides (ZnZrOx) are highly selective and stable catalysts for the hydrogenation of CO2 to CH3OH. However, their catalytic activity has remained relatively moderate, and the influence of the ZnZrOx crystalline phase on performance is not yet fully elucidated. Here, we report a mixed-phase ZnZrOx, comprising coexisting tetragonal and monoclinic domains, and correlate this biphasic architecture with the catalytic performance. At 320 °C, the mixed-phase ZnZrOx catalyst delivers a CO2 conversion of 9.2% coupled with an impressive CH3OH selectivity of 87%, representing a 1.4-fold increase in conversion compared to its purely tetragonal counterpart while maintaining equivalent selectivity. In-depth characterizations attribute this improved performance primarily to the emergence of a two-phase interface, which enhances the dissociation and activation of H2. Density functional theory calculations further reveal that this interfacial region plays a vital role in promoting heterolytic H2 dissociation, boosting the formation of HCOO* and lowering the energy barriers of the rate-determining step for CH3OH formation. This work highlights the effectiveness of the crystal-phase architecture in optimizing ZnZrOx catalysts for CO2 hydrogenation to CH3OH, offering strategic insights for the design of advanced oxide-based hydrogenation systems.
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MOLECULES
·
2025
·Vol. 30
·期 17
·3475
·
IF 4.6
Xiaoqian Xu,Song Yang,Yixiang Wang,Ying Chen,Assa Aravindh Sasikala Devi,Feng Hu
Silver is a promising electrocatalyst for electrochemical CO2reduction reaction owing to its high selectivity and efficiency for CO production. However, it still faces a fundamental trade-off between reaction activity and stability. Here, we developed a three-dimensional coral-like porous silver (CP-Ag) catalyst through seed-assisted nanoparticle attachment synthesis, which creates a unique architecture featuring interconnected pores and stable grain boundaries (GBs) between constituent Ag nanoparticles (Ag NPs). Compared to normal Ag NPs, CP-Ag demonstrates superior catalytic performance, maintaining >90% Faradaic efficiency (FE) for CO across a wide potential range (−0.6 to −1.0 V vs. RHE) while achieving 2-times higher current density. Importantly, CP-Ag demonstrated an impressive long-term stability by sustaining nearly 90% FE for CO approximately 40 h at a current density of −50 mA cm−2in a flow cell. The enhanced catalytic performance arises from three factors: (1) the three-dimensional coral-like morphology increases accessible active sites and promotes charge transfer efficiency; (2) stable GBs between interconnected nanoparticles increase reaction activity; (3) more moderate binding on Ag (100) preferentially promotes *CO intermediate formation. Our findings highlight the importance of simultaneously engineering both morphological and crystallographic features to optimize silver catalysts for CO2conversion.
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JOURNAL OF POLYMER RESEARCH
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2025
·Vol. 32
·期 7
·1-15
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IF 2.8
Liu Li,Zhao Shuaishuai,Liu Jinxin,Zhan Ende,Wei Jinyun,Xing Mengyi
CO 2 flooding, as an effective method for developing low-permeability heavy oil reservoirs, is often limited by the early gas breakthrough due to the high mobility of the gas. To address this issue, research on enhanced oil recovery using a composite flooding method combining viscosity reducer and CO 2 was conducted. Firstly, a novel low molecular weight viscosity reducer, PAINS, was prepared. Subsequently, the mechanism of viscosity reduction by the viscosity reducer in heavy oil was explored from a molecular simulation perspective. Finally, the oil displacement efficiency of the viscosity reducer-CO 2 combination flooding was studied through core flooding experiments. The results showed that the prepared viscosity reducer exhibited effective viscosity reduction; within the viscosity reducer-heavy oil system, the viscosity reducer achieved its effect by altering the internal structure of the heavy oil. The slug of the viscosity reducer was able to improve the mobility ratio of oil and gas caused by viscosity differences, delaying the breakthrough of CO 2 along gas flow channels. The viscosity reducer-CO 2 combination flooding method increased oil recovery by 14.5% compared to single CO 2 flooding, indicating that the viscosity reducer-CO 2 combination flooding technology has broad application prospects in the development of low-permeability heavy oil reservoirs.
Section
Graphical abstract
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Sustainable Materials and Technologies
·
2025
·
IF 9.2
Shiyu Huang,Deqi Fan,Chengxiao Zhao,Xin Li,Xiaofei Yang
The photocatalytic conversion of anthropogenic carbon dioxide (CO 2 ) into solar fuels using semiconductor nanomaterials represents a promising and sustainable approach to addressing both energy sustainability and climate change concerns. Developing highly efficient semiconductor-based photocatalysts to tailor reaction pathways of CO 2 reduction is the key to producing value-added products with desirable performance. Herein, we report a novel copper-doped indium oxide (Cu-doped In 2 O 3 ) nanostructure prepared via the electrospinning technique, followed by annealing to enhance photocatalytic CO 2 reduction. Our findings demonstrate that modifying the bulk In 2 O 3 with copper enables Cu-doped In 2 O 3 nanofibers to catalyze the CO 2 reduction reaction more efficiently. In situ FTIR spectra measurements were utilized to identify the reaction intermediates and gaseous products for validating the reaction pathway. Combined with in situ electron paramagnetic resonance (EPR) and vibrational spectroscopy measurements, which revealed that interstitial Cu doping induces lattice distortions and oxygen vacancy (O V ) formation, effectively enhancing visible light absorption, accelerating charge separation, and migration. Consequently, the optimized In 2 O 3 -Cu3% nanofiber photocatalyst demonstrated outstanding selectivity (100 %) and a CO production rate of 45.5 μmol·g −1 ·h −1 , which is approximately six times higher than In 2 O 3 . Mechanistic studies have indicated that O V defects serve as electron reservoirs to suppress the recombination of photogenerated charges, while simultaneously creating abundant CO 2 chemisorption sites in nanostructures.
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ADVANCED MATERIALS
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2025
·
IF 26.8
Cunbao Huo,Shuwang Wu,Rongjiang Zhang,Zhiqiang Wu,Xiaoyong Tian,Lei Tan,Kexin Li,Yao Yang,Baojie Wang,Zhun Hu,Lingling Wu,Dichen Li
Conventional packed-bed catalysts suffer from single-scale porosity, insufficient mechanical strength, and suboptimal mass transfer efficiency. Inspired by the fractal structure of the lung bronchi, a design and 3D printing method for gradient meta-structural catalysts is proposed by integrating synthesized LaFe 0.5 Ni 0.5 O 3 (LFN) perovskite with pseudo-boehmite, achieving ultralow pressure drop and high catalytic efficiency. Computational fluid dynamics and reaction simulations guide the design of uniform and gradient-structured catalysts with hierarchical woodpile channels (0.5–3 mm). Compared with homogeneous catalysts, the gradient design theoretically exhibits 1.5-fold and 1.1-fold increases in flow velocity and hydrogen production, respectively. Meta-structural catalysts are fabricated with gradient multi-peak pore distribution (9.32 nm, 103.75 nm) by regionally modulating unit cell sizes and LFN content (11–35%) combined with the dehydroxylation of pseudo-boehmite. 3D-printed perovskite catalysts demonstrate a 78.7-fold increase in specific surface area (102.26 m 2 g −1 ) and compressive strength of 8.48 MPa. In dry reforming of methane (DRM) tests, it achieves 82.13% CH 4 conversion, and 9.69 mmol g −1 syngas yield, outperforming conventional powder-packed beds by 10% efficiency. This study achieves mass transfer and catalytic performance coupling by tuning gradient hierarchical pores and tailoring flow dynamics, offering a paradigm for robust, high-efficiency catalyst design across diverse applications.
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