Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123407
·
IF 7.5
Inam Ullah,Syed Musab Ahmed,Hao Lou,Zeeshan Abbasi,Zubair Ahmad,Muhammad Usman,Wenlong Wu,Zhandong Wang
The practical application of CO 2 methanation is often hindered by water-induced limitations. Conventional sorbent-assisted catalyst systems employ adsorbents merely as passive water scavengers, neglecting their potential role in reaction kinetics. Herein, we report a layer-by-layer catalyst-zeolite architecture that overcomes these limitations by synergistically promoting low-temperature CO 2 activation while enabling effective in-situ water management. This ordered configuration maximizes interfacial contact, allowing the hydrophilic NaA zeolite to actively capture and activate CO 2 at reduced temperatures while continuously removing the water by-product from the Ni/ZrO 2 surface. Consequently, the system achieves 81% CO 2 conversion with 100% CH 4 selectivity at 200 ℃. This work demonstrates that integrating Ni/ZrO 2 catalyst with a functional NaA zeolite provides an energy-efficient and robust strategy for sustained low-temperature CO 2 methanation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Meigui He,Jiangquan Chen,Xiaodong Zhang,Chang Chen,Mengfan Ren,Jing Zhao,Wanqin Jin
Ultrathin mixed-matrix membranes (MMMs) have emerged as promising candidates for efficient membrane-based carbon capture, owing to the combination of the high performance of mixed-matrix materials, and the low mass-transfer resistance of ultrathin membranes. However, incorporating fillers into ultrathin separation layers remains challenging due to the strict requirements on filler dimension and dispersion. Herein, we report a Pebax-based ultrathin MMM incorporating ZIF-8@COF composite porous nanosheets for efficient CO 2 /N 2 separation. Ultrasmall ZIF-8 nanoparticles (∼4 nm) were grown in situ on COF nanosheets, yielding a composite porous filler (∼11 nm thick) that combines the high aspect ratio of COFs with the superior interfacial compatibility and CO 2 affinity of ZIF-8. The resulting ZIF-8@COF/Pebax membrane exhibits 63% and 41% enhancements in CO 2 permeability and CO 2 /N 2 selectivity, respectively, over the pristine Pebax membrane, which can be attributed to abundant CO 2 adsorption sites from ultrasmall ZIF-8, well-defined molecular transport pathways from the porous nanosheets, and hydrogen-bond-mediated interfacial chain rigidification. Remarkably, the separation layer remains defect-free even when thinned to ∼100 nm, owing to the ultrathin architecture of the ZIF-8@COF nanosheets and their excellent interfacial compatibility. The resulting ultrathin mixed matrix membrane delivers an attractive CO 2 permeance of 1365 GPU and a CO 2 /N 2 selectivity of 38.4 under mixed-gas conditions, along with robust operational stability and pressure resistance. This work demonstrates that two-dimensional porous composites hold great promise as fillers for fabricating high-performance ultrathin MMMs toward practical carbon capture applications.
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Membranes
·
2026
·Vol. 16
·期 6
·189
·
IF 4.2
Huimin Ma,Xiaoxue Jiang,Nianwei Man,Jing Zhao
The urgent demand for energy-efficient CO2separation technologies has propelled significant advancements in polymer-based CO2separation membranes over the past decade. This review systematically examines three primary classes of these membrane materials: conventional dense polymer membranes, microporous polymer membranes, and mixed matrix membranes (MMMs). We analyze their distinct transport mechanisms, advantages, and the persistent challenges of permeability-selectivity trade-offs, physical aging, and scalability that have hindered widespread industrial adoption despite significant laboratory advances. Furthermore, we offer a forward-looking perspective on critical research directions, including the molecular design of stable microporous polymers, the evolution of MMMs towards continuous hybrid architectures, and the development of scalable ultrathin membrane fabrication techniques. By integrating materials innovation with engineering practicality, polymer-based membranes are poised to play a transformative role in sustainable carbon management.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Jing Zhang,Yutong Dai,Songyao Liu,Can Fang,Jingru Yang,Xianyi Ma,Linjie Ye,Jiqing Lu,Yubing Xiong,Zhifeng Dai
To address the challenges associated with global carbon emissions, this study developed a novel class of porous ionic polymer catalysts. Using a bipyridine-based porous organic polymer (POP-Bpy) as the framework, two Ionic liquid-functionalized materials, POP-Bpy-Et and POP-Bpy-OH, were successfully synthesized via quaternization with 1,2-dibromoethane and 2,3-dibromopropanol, respectively. Comprehensive structural characterization (including 13 C NMR, FTIR, and XPS) confirmed the successful quaternization and formation of the desired ionic polymer architectures. Catalytic evaluation revealed that POP-Bpy-OH exhibits outstanding performance in the cycloaddition of CO 2 with epoxides. Under mild conditions (60 °C, 1 atm CO 2 , 48 h), POP-Bpy-OH achieved 94.3% conversion of epichlorohydrin with 99% selectivity toward the corresponding cyclic carbonate, significantly outperforming the hydroxyl-free counterpart POP-Bpy-Et (78.4% conversion). Moreover, under industrially relevant low-CO 2 conditions (15 %CO 2 , 96 h), POP-Bpy-OH maintained a high conversion of 83.3%, far exceeding that of POP-Bpy-Et (64.2%). This enhanced activity is attributed to a pronounced synergistic effect between the hydroxyl groups (acting as hydrogen-bond donors) and the bromide anions (Br − ) in POP-Bpy-OH, which not only boosts reaction efficiency but also affords good substrate compatibility for epoxides with low to moderate steric hindrance. These results underscore that incorporating hydroxyl functionalities into the polymer backbone is a key strategy for improving CO 2 cycloaddition catalysis. In addition to high activity, POP-Bpy-OH demonstrated excellent structural stability and recyclability. After five consecutive reaction cycles, its catalytic activity decreased by only about 3%, highlighting its potential for practical industrial application. To elucidate the origin of its superior performance, density functional theory (DFT) calculations were employed to probe the reaction mechanism. The simulations show that the hydroxyl groups lower the ring-opening energy barrier of the epoxide via hydrogen-bonding interactions, while the adjacent Br − facilitates the nucleophilic attack. This cooperative action efficiently drives the cycloaddition reaction forward, providing an atomic-level understanding of the catalyst's high activity and selectivity.
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Journal of the American Chemical Society
·
2026
·
IF 16.6
Hou Tianfeng,Tang Tongming,Feng Yuhua,Yang Qingzhuoma,Wei Jinman,Wang Lin,He Donghao,Chen Zhen,Hu Jianjun,Zeng Cuiping,Yu Tao,Wang Bo
Carbon-negative biomanufacturing is essential for global
sustainability.
Artificial photosynthesis based on material-microbe hybrid systems
holds promise but suffers from inefficient energy supply, phototoxicity,
abiotic–biotic incompatibility, and limited product spectrum.
Here, we present artificial photosynthetic hydrogel microspheres (APHM)
as a versatile platform for efficient and programmable CO 2 valorization. Within an alginate/carboxymethyl cellulose hydrogel
matrix, spatial compartmentalization integrated a COF/Pt/Cr 2 O 3 photocatalyst (for in situ hydrogen evolution) and
a light-shielded acetogen ( Acetobacterium woodii ) in a tailored bifunctional medium, enabling CO 2 -to-acetate
conversion. The system operated stably under high-intensity illumination
(60 mW cm –2 ), achieving a near-stoichiometric H 2 -to-acetate coupling efficiency of 88.85%. The resulting acetate
served as a well-defined carbon hub, enabling seamless interface with
engineered yeast for programmable synthesis of diverse products, including
glucose (316 mg L –1 ), myo -inositol
(64 mg L –1 ), glucosamine (24 mg L –1 ), sucrose (609 mg L –1 ), and starch (256 mg L –1 ). Overall, this work presents a universal, efficient
route to versatile solar-to-chemical synthesis.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Tianyi Li,Xing Liu,Yudong Li,Gongwei Tian,Haiyue Yang,Chengyu Wang
To overcome the limitations of traditional binary sulfide photodegradation and charge recombination, ternary metal sulfide solid solutions provide a promising solution through atomic-level bonding reconfiguration, continuous electron distribution, and the synergy of dual metal sites. In the present study, a Cu 3 SbS 4 solid solution photocatalyst was successfully synthesized via a hydrothermal approach, exhibiting superior performance in the photoreduction of CO 2 , demonstrating high selectivity for the conversion of CO 2 to CO and CH 4 , with yields of 1.8083 mmol g –1 and 0.4232 mmol g –1 , respectively, over a 5-hour reaction duration, alongside excellent cycling stability. Combining in situ spectroscopy with DFT calculations, the enhanced photocatalytic activity of Cu 3 SbS 4 stems from the cooperative bonding effect within its molecular framework. Specifically, the Cu–S bonds form a continuous low-energy barrier path, facilitating electron localization and inhibiting interphase carrier recombination, while the Sb–S bonds construct local active sites on the surface, facilitating CO 2 adsorption and activation. The Electron Localization Function (ELF) analysis indicates that this solid solution overcomes the discontinuous, island-like electron distribution characteristics in the binary system, forming a uniform and continuous network of electron localization, significantly reducing the in situ recombination centers. The synergistic action of the bimetallic (Cu/Sb) sites reduces the key reaction energy barriers, and local lattice distortion exposes high-activity surface sites. Additionally, the elongation of the Cu–S bonds increase the oxidation energy barrier of sulfur, effectively alleviating photodegradation. This study provides atomic-scale evidence for the rational design of bonding cooperation in multi-component sulfide solid solution photocatalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 34
·18159-18168
·
IF 3.9
Ren Xuping,Zhao Zijiang,Long Yanhui,Zhang Wenjun,Wang Jun,Zhang Hao
Developing efficient catalysts for
CO 2 hydrogenation
to methanol remains a challenge due to the inherent trade-off between
activity, selectivity, and cost. Herein, a series of metal-promoted
Cu catalysts (Zr, Zn, Ga) were synthesized via a ligand-modulated
oxalate coprecipitation strategy using malachite-derived CuO as the
precursor, enabling a low-cost and sustainable catalyst design. Among
these, the ZrO 2 /Cu catalyst (Zr/Cu = 14:86) exhibits the
optimal performance, delivering a CO 2 conversion of 13%
and a methanol space-time yield (STY) of 280.1 g MeOH ·kg cat –1 ·h –1 at 280 ° C
and 3.0 MPa, together with excellent long-term stability. Characterization
results suggest that highly dispersed Zr species effectively suppress
Cu particle agglomeration while generating abundant surface oxygen
vacancies (O V , 43.5%). Mechanistic studies indicate that
Zr incorporation induces strong electronic metal–support interactions
(EMSI), leading to the formation of electron-rich Cu 0 /Cu + sites. These sites act cooperatively with O V ,
where the former facilitates H 2 dissociation and the latter
promotes CO 2 adsorption and activation. Such synergistic
effects favor the formate-mediated pathway while suppressing the competing
reverse water–gas shift reaction. This work not only demonstrates
a high-performance catalyst derived from natural minerals but also
provides insights into the atomic-level synergy between electron-rich
metal sites and surface defects, offering a viable strategy for the
rational design of efficient catalysts for CO 2 hydrogenation.
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Green Chemical Engineering
·
2026
·
IF 11.9
Xin-Yi Yang,An-Guo Wu,Fang-Yu Yu,Li-Feng Xu,Guang-Rui Liu,Hong-Ru Li,Liang-Nian He
In this work, a “CO 2 capture and ex situ utilization” strategy was proposed by combining calcium looping and a subsequent cycloaddition reaction. In the calcium looping step, the CaO-based sorbent was prepared from bulk industrial solid waste, i.e., carbide slag as the calcium source and blast-furnace slag as the dopant. Both wet mixing and sol-gel methods were explored in this study. Among them, the sorbent synthesized via the sol-gel route with sucrose as a complexing agent showed improved cyclic performance. This improvement is presumably attributable to the sol-gel method's ability to enhance the distribution of blast furnace slag and optimize the sorbent's pore structure. By further regulating sorbent preparation parameters such as the mass ratio of carbide slag to blast furnace slag, the sucrose amount, and the calcination temperature and time, the optimal sorbent was obtained with an initial CO 2 uptake of 0.552 g CO 2 /g sorbent at 740 o C. Furthermore, the CO 2 uptake was still retained at 92% even after 10 cycles. The CO 2 released from Ca-looping ex situ reacted with propylene oxide (PO) to afford a 91% yield of propylene carbonate catalyzed by graphene oxide (GO) and tetrabutylammonium bromide (TBAB), avoiding conventional CO 2 compression and transportation. As expected, this study represents a potential large-scale application of integrating industrial solid waste management, carbon capture, and valorization to value-added chemicals and materials.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Sun Mingyang,Hu Ziyan,Liu Yilang,Lv Chenyan,Zhang Tuo,Zhao Guanghua,Zang Jiachen
Efficient noble-metal-free photosynthesis systems for CO 2 conversion based on earth-abundant elements have been largely unexplored. On the other hand, large quantities of bovine blood as waste byproducts during meat processing pose environmental challenges. To address these concerns, herein we report a biomimetic photocatalytic platform constructed by hemoglobin, a major component in bovine blood, which structurally and functionally emulates the fibrous chloroplasts of Spirogyra . Under denaturing conditions, hemoglobin molecules self-assemble into heme-containing amyloid-like fibrils, in which the intrinsic heme groups serve as visible-light photosensitizers. Subsequently, iron-based catalytic cores are uniformly deposited along the protein fibrils, generating a hierarchical architecture that integrates heme as a light-harvesting domain and iron cores as catalytic functionalities within a single scaffold. This spatially organized system effectively shortens electron transfer distances and promotes interfacial charge migration. Consequently, the as-prepared biomimetic assembly exhibits efficient visible-light-driven CO 2 reduction to formic acid with high activity and selectivity as compared to conventional homogeneous systems. Notably, this work not only provides a noble-metal-free strategy for constructing integrated photocatalytic systems but also demonstrates a viable pathway for transforming biological waste into high-value functional materials.
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Carbon Capture Science & Technology
·
2026
·
IF 10.2
Ali A. AL-Thuraya,Wen He,Jingcheng Du,Pengjia Dou,Qian Sun,Ayan Yao,Xuan Ding,Daijun Meng,Jiangtao Liu
Polymeric membranes for CO 2 capture often face a trade-off between permeability and selectivity. Here, crown ethers were introduced as molecular shuttles for CO 2 transport by in situ encapsulation within ZIF-8 nanocages. Three crown ethers (18-crown-6 (18C6), diaza-18-crown-6 (DAC), and dibenzo-18-crown-6 (DBC)) were incorporated into ZIF-8 during crystallization and then used as low-loading fillers in Pebax mixed-matrix membranes. Structural characterization by XRD, FTIR, SEM/EDS, and BET confirmed that ZIF-8 crystallinity was preserved, while pore volume, linker rotation, and filler dispersion were effectively tuned. These modifications narrowed transport pathways and strengthened polymer–filler interactions, improving CO 2 separation performance. At an optimal loading of 1 wt% 18C6@ZIF-8, the membrane doubled CO 2 permeability relative to neat Pebax and increased CO 2 /N 2 selectivity from 55.5 to 85.8, surpassing the 2008 Robeson upper bound. The membrane also maintained stable performance under feed pressures up to 20 bar and exceeded the 2019 Robeson upper bound. Mixed-gas testing showed a CO 2 permeability of 158.3 Barrer and CO 2 /N 2 selectivity of 66.0, outperforming neat Pebax. Transport analysis revealed that the enhancement mainly arose from improved diffusion selectivity, with a minor contribution from solubility selectivity. Among the fillers, 18C6@ZIF-8 provided the best permeability–selectivity balance, demonstrating a promising strategy for advanced CO 2 -selective mixed-matrix membranes. This approach paves the way for the development of next-generation mixed-matrix membranes (MMMs) with enhanced performance for CO 2 capture and a range of other gas-separation applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Tong Huang,Qiuyu Wu,Dong Qi,Feifan Yang,Yaqiong Xie,Guangru Zhang,Xin Liu,Gongping Liu,Haipeng Zhu
Natural gas upgrading demands advanced CO 2 /CH 4 separation membranes for CO 2 removal. Polymer of intrinsic microporosity (PIM-1) represents a novel polymeric molecular sieve featuring exceptional permeability and processability, but its moderate CO 2 /CH 4 selectivity remains challenging. Plasma treatment, a well-applied technique for surface modification of dense polymers, has been adopted to PIM with abundant interchain micropores for the first time. The physical alteration of plasma treatment in He gas atmosphere, primarily the chain scission, has significant impacts on CO 2 /CH 4 separation performance of PIM-1 membrane, by means of regulating its hierarchical microporous structure. Wide angle X ray scattering (WAXS) results suggest that the relatively large micropores are more prone to shrinkage and collapse than relatively small ones, which effectively enhances the selectivity. Moreover, owing to near-surface localization effect, the plasma modification is constrained within a skin layer onto a bulk intact layer. This asymmetric membrane structure allows the balance of enhancing CO 2 /CH 4 selectivity and sustaining high CO 2 permeability. By optimizing plasma input power and duration, the selectivity of plasma-treated PIM-1 membrane increased by 1.65 times, with a high permeability of over 4000 Barrer. After 2-month aging, the permeability was still maintained 60 % of its initial value. This suggests plasma treatment as a promising post-modification method for PIM CO 2 /CH 4 separation membranes.
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CRYSTAL GROWTH & DESIGN
·
2025
·
IF 3.4
Yingying Liu,Lintao Sun,Huazheng Xu,Xuening Ma,Jiani Ren,Lanlan Jiang,Jia-nan Zheng,Yongchen Song
Crystal growth characteristics determine the formation of carbon dioxide (CO2) hydrate. This study experimentally realized the regulation of CO2 hydrate growth mode from multidimensional to one-dimensional based on multiphase transportation theory inside porous media and succeeded visually observing the ray type growth process of many hydrate crystals at the interface between bulk gas and porous media. There are a few nucleation points in each experimental case, and from which the hydrate bud crystals of approximately 0.74 mm in diameter grow above on the porous media, reaching 26 mm long at most. Analysis of mass transfer within porous media revealed that the continuous growth of hydrate buds is driven by water self-transportation among pores. That is why that either large particle (over 0.8 mm diameter) or low water saturation (less than 30%) inhibits the effective growth of hydrate buds. In particular, by dynamic tracking in continuous images, the growth rates under different water saturation and particle size conditions are quantified, and the one-dimensional growth rate of hydrate is determined as 0.04 mm/s. This study unveils the mystery growth mechanism of CO2 hydrate for the first time and is extremely significant to future researches on the fundamental and application of various gas hydrates.
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