CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Meiling Ran,Li Fan,Yangyang Yu,Jiawei Xie,Sheng Qiu,Lei Song,Chao Wang,Kui Ma,Hairong Yue,Chang-An Zhou
Electrochemically mediated carbon capture (EMCC) based on redox-active CO 2 carries is regarded as a promising pathway for carbon capture under mild conditions. Owing to their reversible electron-transfer capability, quinones have been widely researched in aqueous EMCC systems. However, their highly symmetric structure severely restricts solubility, which adversely affects the electrochemical efficiency and stability in non-aqueous systems. Here, we introduce sulfonate groups (–SO 3 − ) into the anthraquinone molecule to modulate the molecular polarity and suppress π-π stacking, significantly improving solubility and optimizing capture performance. Research revealed that 2-AQS exhibits optimal solubility, viscosity, conductivity, and electrochemical properties. During the 120 h of electrochemical CO 2 capture, it maintained a capacity retention rate of 76.35% and a coulombic efficiency of 85.06%, with an energy consumption of 285.92 kJ·mol −1 , markedly lower than that of unmodified AQ (498.23 kJ·mol −1 ). This work reveals the impact of sulfonate functionalization on the EMCC performance of anthraquinone derivatives, providing a balanced and cost-competitive candidate (2-AQS) for practical EMCC applications.
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ACS Catalysis
·
2026
·
IF 13.6
Shan Tang,Qingnan Wang,Siyu Chen,Xiaohong Li,Lanqi Ning,Ruizhi Duan,Jijie Wang,Can Li
CO2 hydrogenation to methanol utilizing renewable H2 offers a promising route for carbon neutrality, but efficient catalysts with synergistic active sites of H2 and CO2 remain challenging. Herein, we demonstrate a TiO2-supported rhenium-zinc binary oxide catalyst that exhibits methanol selectivity up to ca. 70% at a CO2 conversion of 9.3% and a methanol space-time yield of 529 mg·h−1·gcat−1 at 320 °C and 5 MPa, outperforming ReOx/TiO2 and ZnO/TiO2 catalysts by 5.8 and 2.3 times, respectively. Kinetics analysis combined with structural characterization supports the synergistic effect between dual ReOx and ZnO sites for enhanced performance. Strong Re-Zn interactions generate ReOx sites that are responsible for promoted H2 activation, whereas the highly dispersed, partially reduced ZnO strengthens CO2 adsorption and activation. The activation of CO2 and H2 is decoupled on distinct sites yet coupled via efficient hydrogen supply, thereby accelerating hydrogenation of CO2-derived intermediates. In situ diffuse reflectance infrared Fourier transform spectroscopy reveals a preferred formate pathway, featuring the evolution of b-CO3* to HCOO* and subsequently to H3CO*. This work highlights the synergistic effect between dual oxide sites in promoting selective CO2 conversion to value-added chemicals.
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Journal of Materials Chemistry A
·
2026
·
IF 9.2
Jiayou Liao,Shouwei Liu,Xinyue Meng,Chengyun Gao,Xianjie Meng,Zhichao Zhai,Shuangming Wang,Yong Wang,Xu Wu,Jinping Li
Capturing low-pressure CO2 from industrial flue gas is challenging due to the trade-off between permeability and selectivity in polymeric membranes. To address this issue, we reported a surface engineering strategy to fabricate high-performance asymmetric hollow fiber membranes (AHFMs) with an amine-functionalized surface-localized ultra-thin functional layer. We utilized a brominated 6FDA-DAM polyimide precursor to fabricate AHMs via spinning, where bromine groups disrupt polymer chain packing to optimize bulk diffusion pathways, while simultaneously serving as reactive sites for nucleophilic substitution. By grafting polyamines onto the membrane surface, we successfully established a facilitated transport layer via surface reactions on the surface-localized ultra-thin functional layer. This design synergizes the fast permeation of the solution-diffusion bulk with the high affinity of the facilitated transport surface. In comparison with the pristine membrane, the amine-grafted membrane exhibited a simultaneous enhancement in separation performance. Under single-gas conditions at 0.2 MPa, the CO2 permeance of the membrane can reach 1362 GPU and the ideal CO2/N2 selectivity can reach 65, representing 1.33 times and 1.38 times increases over the pristine PI-Br-70% membrane, respectively. This demonstrates the efficacy of the surface functionalization strategy. Furthermore, the chemically cross-linked surface provides structural rigidity that effectively suppresses CO2-induced plasticization. The membrane also ensured stable separation performance over 1440 h of continuous operation. This study presents a reliable method for developing scalable membranes with high flux and durability for energy-efficient carbon capture.
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
·
2026
·
IF 17.6
Shuaiqi Gong,Chuxiong Zhou,Xiaoyang He,Jianying Wang,Penghui Shi,Yulin Min,Zuofeng Chen,Hexing Li
Photocatalytic CO 2 reduction to ethanol (C 2 H 5 OH) offers a sustainable carbon recycling route but is limited by inefficient C−C coupling under visible light irradiation. Here, we report a defect-engineered WO 3-x /In SAs (SAs, single atoms) photocatalyst with a dynamic dual-site relay mechanism, where electron-rich W−V O (V O , oxygen-vacancy) and electron-deficient In single atom sites cooperatively drive selective ethanol synthesis. The W−V O site acts as a persistent *CO supply hub for CO 2 -to-*CO conversion, while In site functions as an ethanol-selective coupling center for targeted *CO−*CO coupling. This relay enables exceptional ethanol production and high selectivity (97.43% electrons selectivity and 86.35% yield-based selectivity). Notably, the photocatalyst maintains efficient CO 2 -to-ethanol conversion efficiency under natural sunlight illumination in scaled-up experiments using a reactor equipped with a 20 × 20 cm 2 plate coated with WO 3-x /In SAs . Combined in situ spectroscopy and DFT calculations reveal that W−V O orchestrates CO 2 -to-*CO feeding and relays electrons to In SAs , reducing the C−C coupling barrier via asymmetric electron distribution. Electron-trapping at oxyphilic In stabilizes *CO via O-lone-pair donation; subsequent W d-orbital hybridization anchors *OCCO, dictating ethanol selectivity. Our work provides a design strategy for efficient photogenerated carrier utilization in CO 2 -to-ethanol conversion, with implications for scalable solar fuel synthesis. Graphical Single-atom In-decorated defective WO 3-x establishes a dynamic dual-site relay for selective CO 2 photoreduction. Oxyphilic In traps electrons to anchor *CO via O-donation, while adjacent W sites facilitate *OCCO formation through d-orbital hybridization. This synergy directs C−C coupling and selective hydrogenation, achieving 86.35% ethanol selectivity without sacrificial agents.
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Science Advances
·
2026
·Vol. 12
·期 29
·
IF 13.9
Qixing Zhang,Jing Gao,Muchen Li,Ying Yang,Guanlan Chen,Han He,Xingfei Chen,Xiaobing Gu,Yajun Gao,Yongcai He,Bo He,Xixiang Xu,Zhenguo Li,Ying Zhao,Lijun Zhang,Michael Grätzel,Xiaodan Zhang
Solar-driven electrochemical CO 2 reduction to multicarbon (C 2+ ) products presents a promising avenue for artificial photosynthesis, yet remains constrained by high overpotentials and limited conversion efficiency. Here, we developed an alkaline environment-modulated prereduction strategy that capitalizes on the divergent thermodynamic stabilities of precursors, enabling the precise synthesis of iodine-doped copper nanotopologies (Cu-I NTs). Featuring tunable under-coordination defects and stabilized high-energy adsorption sites, the Cu-I NTs achieve an onset potential of only −0.37 V versus the reversible hydrogen electrode for C 2+ formation. Operando Raman measurement and density functional theory calculation reveal that the tailored surface topologies favor Cu-CO rotation adsorption, enabling dynamic reorientation from bridge- to atop-binding configurations, which collectively lowers the barrier for CO-CO coupling. Impressively, powering the electrolyzer by a perovskite/silicon tandem together with a single-junction silicon photovoltaic device, the system delivers a photocurrent of 12.34 mA cm −2 at 2.17 V under standard AM 1.5 illumination, achieving a solar-to-C 2+ conversion efficiency of 8.64%.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2026
·Vol. 227
·期 15
·e70321
·
IF 2.8
Baihu Dong,Haoyuan Sun,Xiang Wang,Yunqi Chen,Xinqiang Wang,Yingfeng Tu,Shaohui Lin,Qinmin Pan,Xianshe Feng,Flora T. T. Ng
A novel polystyrene-supported Salen-cobalt(III) complex (PS-Salen-Co(III)-OAc) is prepared via covalent immobilization onto functionalized polystyrene microspheres. The catalyst is comprehensively characterized by FT-IR, XPS, SEM-EDS, and ICP-OES, confirming successful immobilization and preservation of the catalyst sites. This heterogeneous system is applied in the alternating copolymerization of carbon dioxide (CO 2 ) and propylene oxide (PO), achieving high polycarbonate yields (up to 76%), excellent chemoselectivity (up to 99%), and narrow molecular weight distributions in the presence of a chain transfer agent ( Ð as low as 1.04) under mild conditions (30°C, 500 psi). The introduction of 1,2-propanediol as a chain transfer agent further enhances the control over molecular weights. However, catalyst reuse is hindered by substantial mass gain due to covalent grafting of the polycarbonate product onto the supporting polystyrene matrix via the surface hydroxyl groups. Attempts to mitigate this grafting through hydroxyl capping and reduction are partially effective. A degradation-recycling strategy, based on controlled depolymerization of surface-grafted polymer chains via a back-biting mechanism, significantly reduces mass gain and restores catalytic activity in subsequent cycles. This study provides a practical and efficient platform for sustainable CO 2 utilization through regenerable heterogeneous catalysis.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2026
·
IF 3.1
Tao Zhu,Anqi Ming,Yuxiang Cao,Wencong Li,Xiaoxiao Li,Jun Sun,Lin Chen
CO 2 -responsive cationic polymers offer a route to couple industrial kiln exhaust pretreatment with sludge deep dewatering, using the abundant CO 2 in flue gas as a trigger to enhance flocculation. This study proposes a flocculation then activation strategy to enhance the flocculation effects of the CO 2 -responsive Poly-(DMC-DMAEMA) copolymer. The polymer is first dispersed in its low-viscosity, non-activated state to achieve uniform contact with suspended particles, followed by CO 2 bubbling to trigger in situ protonation of the PDMAEMA blocks. Using a diatomaceous suspension as model sludge, flocculation behaviors under different CO 2 addition modes were systematically compared. Pre-activation caused a sharp increase in solution viscosity and poor dispersibility, aggravating inhomogeneity. Post-activation-dispersion followed by CO 2 activation effectively balanced uniform adsorption with in situ bridging reinforcement, yielding superior floc growth, turbidity removal, and dewatering efficiency. This mechanistic strategy directly resolves the dispersion problem characteristic of conventional high-molecular-weight flocculants, thereby establishing a foundation for the integrated application of kiln exhaust pretreatment and sludge deep dewatering.
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AICHE JOURNAL
·
2026
·
IF 4.4
Chaodi Jin,Heli Tian,Ruoyu Hu,Beiqi Sun,Xing Hu,Min Xiao,Hongxia Gao,Teerawat Sema,Zhiwu Liang
Liquid–liquid phase separation is an interesting phenomenon that generates two immiscible liquid phases during CO 2 absorption or temperature swing. It provides a promising opportunity to optimize CO 2 capture processes and reduce the energy penalty for solvent regeneration. However, precise control of phase behavior remains challenging. This work achieves controllable phase separation in amine-ether-water systems. Results show that adjusting the ether-to-water mass ratio enables the correlation between critical CO 2 loading and temperature to reversibly shift from negative to positive. This rule is verified in various amines and ethers. Synergistic effects of temperature and CO 2 absorption on phase separation are revealed by 13 C NMR and molecular dynamics simulations. This study deepens the understanding of phase separation and offers a theoretical basis for developing high-performance CO 2 absorbents for industrial applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Di Gao,Jian-Zhi Yang,Heng-Yu Wei,Kong-Zhai Li,Min Lin,Xing Zhu
C e-e Zr solid solution formation strengthens the metal-support interaction. • The catalyst reached 79.02% CO 2 conversion and methanation rate 26.35 mmol·g cat −1 ·h −1 . • Dual-role oxygen vacancies enhance charge separation and CO 2 activation. Photothermal Carbon dioxide (CO 2 ) hydrogenation is a promising strategy for solar-fuel production, but its performance is often limited by inefficient charge separation and poor low-temperature activity. Herein, Ni/Ce-Zr solid solution catalysts were developed by introducing lattice distortion to regulate the electronic structure and generate abundant oxygen vacancies. The resulting oxygen vacancies promote charge separation, enhance CO 2 activation, and strengthen the photothermal synergistic effect. Among the catalysts, 20Ni/Ce 0.75 Zr 0.25 O 2 exhibited the best performance, achieving 79.02% CO 2 conversion, over 99.00% CH 4 selectivity, a methanation rate of 26.35 ± 0.05 mmol·g cat −1 ·h −1 , and an apparent activation energy of 16.23 ± 0.70 kJ/mol at 250 °C, while maintaining stable operation for over 180 h. In situ DRIFTS results reveal that abundant oxygen vacancies facilitate the hydrogenation of key intermediates and suppress carbonate accumulation, thereby preventing catalyst deactivation. These findings demonstrate that oxygen-vacancy engineering is an effective approach for improving photothermal CO 2 methanation and provide guidance for the design of efficient solar-driven CO 2 conversion catalysts. Oxygen Vacancy-Mediated Photothermal CO 2 Methanation over Ni/Ce-Zr Solid Solution. Download: Download high-res image (208KB) Download: Download full-size image
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Journal of Energy Chemistry
·
2026
·
IF 15.6
Haoran Jia,Le Lin,Xiaohui Feng,Xiaoyue Wang,Rentao Mu,Qiang Fu
Competitive adsorption between H 2 and CO x ( x = 1, 2) on oxide catalysts represents a primary limitation in hydrogenation reactions, where mutual site blocking suppresses activity and selectivity. This constraint hampers syngas conversion and CO 2 hydrogenation, yet strategies to decouple adsorbates remain elusive. Here, we show that competitive adsorption can be overcome through a partial-site-occupation mechanism that prevents surface saturation and enables independent activation. For a model ZnCr 2 O 4 @ZnO x system, in situ infrared spectroscopy directly reveals the simultaneous adsorption of H 2 with CO or CO 2 , in contrast to the mutually exclusive adsorption observed on pristine ZnO. Kinetic measurements link this decoupling to suppressed inhibition effects and altered reaction orders, driving improved catalytic performance. Density functional theory combined with temperature-programmed analyses further demonstrates that homolytic H 2 dissociation becomes thermodynamically self-limiting, resulting in intrinsically unsaturated surface coverages. These findings indicate competitive adsorption from an inherent constraint to a tunable surface property and establish practical design strategies for cooperative activation in ZnO-based oxide-catalyzed hydrogenation reactions. The ZnCr 2 O 4 -confined ZnO x catalyst decouples the competitive adsorption between CO/CO 2 and H 2 , enabling the co-adsorption and co-activation of these small molecules. Download: Download high-res image (182KB) Download: Download full-size image
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ACS Catalysis
·
2026
·Vol. 16
·期 17
·17145-17155
·
IF 13.6
He Ye,Liu Huiyu,Sheng Jianping,Du Chenyu,Moghadam Majid,Sun Yanjuan,Dong Fan
Halide perovskite nanocrystals are promising photocatalysts for CO 2 reduction due to their strong light absorption, defect tolerance, and tunable excited-state properties, but their practical performance remains limited by tightly bound excitons, rapid charge recombination, and inefficient interfacial electron delivery. Here, we report an anthraquinone (AQ)-modified CsPbBr 3 nanocrystal photocatalyst (CPB/AQ) in which the redox-active π-conjugated AQ ligand functions as an interfacial electron relay and molecular electric-field modulator. Experimental and theoretical analyses collectively reveal that AQ creates an additional interfacial charge-transfer pathway, strengthens the light-induced surface potential difference from 170 to 270 mV, and decreases the exciton binding energy from 44.05 to 40.74 meV. Consequently, CPB/AQ achieves a CO yield of 433.50 μmol g –1 within 3 h under AM 1.5G irradiation, 4.54 times that of pristine CPB, and maintains stable CO evolution during a 25 h test. Isotopic 13 CO 2 tracing verifies that CO originates from CO 2 reduction, while in situ FTIR spectroscopy demonstrates enhanced CO 2 adsorption/activation and accelerated formation of *COOH and *CO intermediates on CPB/AQ. This work highlights molecularly gated interfacial electric-field regulation as an effective strategy for overcoming charge-transfer bottlenecks in perovskite nanocrystal photocatalysis.
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ENERGY & FUELS
·
2026
·Vol. 40
·期 35
·19588-19599
·
IF 6
Li Zhefeng,Cheng Jun,Sun Yunshuyu,Qiu Yi,Lin Zhen,Mao Yuxiang,Xia Rongxin,Zhang Meng
Cu-based
catalysts are promising for CO 2 -to-methanol
conversion, but their activity and stability are usually compromised
by the accumulation of byproduct water. Although physically mixing
hydrophobic additives with Cu-based catalysts can facilitate water
removal, how to regulate the water-removal kinetics in this process,
as well as its impact on the reaction kinetics of CO 2 hydrogenation
to methanol, remains insufficiently understood. Herein, by modifying
the polydivinylbenzene (PDVB) with porosity, we regulate the surface
hydrophobicity of its mixture with a layered double hydroxide (LDH)-derived
CuZnAlMg catalyst, thereby enhancing the water removal kinetics on
the mixed catalyst surface. In contrast to nonporous PDVB, porous
PDVB, with a substantially higher surface area and abundant mesopores,
effectively creates additional H 2 O transfer channels. This
facilitates rapid water removal, which in turn inhibits the oxidation
of Cu nanoparticles and ensures the re-exposure of oxygen-vacancy
active sites for sustained catalysis. Furthermore, water removal also
accelerates the formation and subsequent hydrogenation of intermediates
for higher activity. Consequently, a high space-time yield of methanol
of 519.89 g MeOH kg cat –1 h –1 and a CO 2 conversion rate of 26.35% are
achieved at 5 MPa and 260 ° C. The mixed catalyst exhibits
excellent stability over 200 h of continuous operation. This work
offers a simple yet robust strategy for regulating catalyst hydrophobicity
toward efficient CO 2 hydrogenation to methanol.
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