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.
✓ 已验证
DOI
高影响因子
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.
✓ 已验证
DOI
高影响因子
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.
✓ 已验证
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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%.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Jingce Bi,Yan Qian,Qingfeng Zhan,Huichun Xue,Ningning Liu,Xia Zhang,Zhuopeng Wang,Lin Zhu,Hongzhu Xing,Yide Han
Nickel Metal-Organic Frameworks (MOFs) Ni-BDC (BDC: 1,4-benzenedicarboxylic acid) with coordination-unsaturated metal sites (CUMs) exhibits remarkable CO 2 reduction activity under visible-light irradiation. However, its photocatalytic mechanism remains a challenging due to complex charge-transfer pathways. Herein, a series of CUMs-tunable MOFs (Ni-BDC-D x ) were synthesized via a pyrazine-assisted aqueous-phase strategy for photocatalytic CO 2 reduction. A positive correlation is found between the CUMs density and photocatalytic activity, and Ni-BDC-D 1.0 with highest CUMs density achieves a remarkable CO production rate of 3503.1 μmol·g −1 ·h −1 , which is 5.2 times higher than conventional bulk Ni-BDC. Experimental and theoretical results reveal that CUMs induce the formation of defect level and enhance CO 2 adsorption. The defect level serves as electron trap to promote localized charge accumulation by the optimizing charge transfer pathway. This pathway is achieved by facilitating non-radiative relaxation pathway to inhibit radiative carrier recombination behavior. These findings provide insights into electron transfer mechanism on CUMs-rich Ni-BDC for photocatalytic CO 2 reduction.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2026
·
IF 11.8
Lu Jiang,Yaning Liu,Qinghua Liu,Zhiwei Yang,Miao Ji,Haonan Chen,Xinya Chen,Furong Qiao,Xiao Huang,Gang Lu
Copper (Cu)-based catalysts are widely employed in electroreduction of carbon dioxide (CO 2 ER) because of their cost-effectiveness and versatility in producing multi-carbon products. However, improving the product selectivity, especially toward C 2 species (hydrocarbon containing two carbon atoms), remains a significant challenge. Herein, the microwave-assisted synthesis of copper oxide (CuO) is modulated with ammonium hexafluorophosphate (NH 4 PF 6 ), obtaining thin CuO (ca. 12 nm in thickness) nanosheets with the surface adsorbed with hexafluorophosphate, referred as CuO-PF 6 . This CuO-PF 6 catalyst could help stabilize the key reaction intermediates during CO 2 ER. Therefore, the Faradaic efficiency (FE) of C 2 products (ethylene and ethanol) during CO 2 ER could be improved to 75.8% ± 0.5% in an H-type electrochemical cell. This C 2 FE increases to 82.4% in a flow cell. The improved FE toward C 2 species could be attributed to the PF 6 -modulated electronic structure of Cu surface and stabilization of key reaction intermediates, especially those involving C 2 production. In addition, CuO-PF 6 also demonstrates a high catalytic stability over 10 h. This work provides a deeper understanding of surface modification strategy for CO 2 ER enhancement, promising for designing hybrid electrocatalysts with high efficiency and stability for CO 2 -to-fuel conversion.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Haonan Li,Wa Gao,Kangli Ma,Jian Lei,Olim Ruzimuradov,Akhtam Samiev,Ya Chen,Jingxiang Low,Yue Li
Cocatalyst loading has been extensively adopted in photocatalysis for enhancing photocatalytic performance. However, the sluggish interfacial charge dynamics between cocatalyst and photocatalyst has restricted the wide applications of such a strategy. Herein, we introduce the Ni–N interfacial bonds between lamellar nitrogen-vacancy-rich g-C 3 N 4 /CoNi 2 S 4 nanoparticles (CN-V N /CoNi 2 S 4 ) composite material to bridge the photogenerated charge carrier separation at their interface. Specifically, extended X-ray absorption fine structure analysis reveals that these Ni–N interfacial bonds are originated from the bonding of CoNi 2 S 4 with the nitrogen atoms adjacent to the nitrogen vacancies (V N ) in g-C 3 N 4 . Experimental evidence and theoretical calculations reveal that Ni–N interfacial bonds cannot only cause an intimate contact interface between CN-V N /CoNi 2 S 4 , but also modulate the charge distribution on the CN-V N and CoNi 2 S 4 , further boosting the photogenerated charge carrier separation. More interestingly, this tailored interfacial microenvironment significantly reduces the energy barrier for key intermediates formation while modulates the rate-determining step from *COOH generation to CO desorption, enabling efficient and controllable CO production. This work establishes a methodological framework for engineering advanced photocatalysts, enabling high-efficiency conversion of solar energy into clean fuels.
✓ 已验证
DOI
高影响因子
ACS Applied Polymer Materials
·
2026
·
IF 4.7
Shuyi Li,Shiyuan Cheng,Jumei Wang,Xiaojing Xing,Xinfeng Cheng,Dongqin Bi,Dongfang Qiu,Nam Hoon Kim,Joong Hee Lee,Xuyang Li
Membrane separation technology has great potential for application in gas separation due to its environmentally friendly, efficient, and energy-saving advantages. Polyamide (PA) membrane is an ideal material for efficient separation of CO2 due to its high amine density and excellent CO2 affinity. This work presents a trio-modulated strategy that enhances the CO2 separation performance of PA membranes by modifying the substrate, optimizing the preparation method, and incorporating fillers. Substrate modification facilitates the interfacial polymerization of a polyamide layer on a polysulfone substrate. PA membranes fabricated via vapor–liquid interfacial polymerization typically exhibit a low defect density and superior CO2 separation performance. The incorporation of fillers (γ-cyclodextrin, namely γ-CD) can effectively loosen the microstructure of the PA membrane, and the CO2-philic groups of γ-CD fillers furtherly enhance the selectivity of CO2 through the facilitated transport mechanism. The prepared membranes display excellent CO2 separation performance with CO2/N2 selectivity of 479.5, CO2/CH4 selectivity of 395.9, as well as a CO2 permeance of 4179.8 GPU. The proposed strategy provides a facile and effective route to trio-modulated PA membranes for the study of CO2 separation and can provide a avenue for the development of advanced membrane materials for CO2 separation.
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2026
·
IF 6
Lefei Cao,Fei Qi,Chengfan Fu,Ge Xu,Nan Zhang,Yayun Pu,Xiaosheng Tang,Qiang Huang
Although dielectric barrier discharge (DBD) plasma represents a promising technology for CO2 conversion, its standalone application remains limited by low conversion efficiency, which could be improved via filling a suitable photocatalyst into the plasma reactor. In this paper, the synergistic effect of discharge plasma and Bi12O17Cl2@Cs2SnCl6–Sb0.35 photocatalyst was studied, achieving efficient carbon dioxide conversion. With the help of a photocatalyst, DBD plasma successfully realized the conversion of CO2 and water to CO, methanol, and ethanol. Compared with Cs2SnCl6–Sb0.35, Bi12O17Cl2-10@Cs2SnCl6–Sb0.35 increased methanol and ethanol production by 186 and 80%, respectively. Meanwhile, the conversion of carbon dioxide increased significantly with the presence of water in the plasma-photocatalyst system, achieving a conversion ratio of 35.6%. This boost is attributed to the enhancement of the surface conductivity of the photocatalyst during the plasma discharge, which in turn optimizes the charge transfer process. This paper provides a new idea and a promising technical roadmap for the resource utilization of CO2, which exhibits scientific significance and application potential.
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Yin Chenxu,Sun Zhecheng,Tang Kunlin,Zou Weixin,Wan Haiqin,Liu Zhao-Qing,Dong Lin
Photocatalytic reduction of CO 2 to natural gas using water vapor is a promising strategy for carbon recycling and renewable energy storage. However, the selectivity of current catalysts still remains a big challenge. Herein, we construct IrCu alloys on TiO 2 nanosheets to promote photocatalytic CO 2 to methane with 98.6% selectivity and 7.9% quantum efficiency at 365 nm under non-sacrificial ambient conditions. The performance is competitive with most other reported metal-based photocatalysts. Experimental and theoretical calculations demonstrate that the intensive H 2 O adsorption on Ir/TiO 2 hinders *H transfer, inevitably generating the H 2 by-product. Conversely, hydrophobic Cu effectively optimizes the interfacial hydrogen-bond network on IrCu/TiO 2 , predominantly in H-down configurations for H 2 O adsorption on the asymmetric charge-polarized Cu δ+ -Ir δ- structure, which facilitates the kinetic migration of dissociated *H to *CO-Cu sites, resulting in the reduced energy barrier for the key *CHO intermediate. This finding enables high CH 4 selectivity on IrCu/TiO 2 , deepening our understanding of gas-solid interfacial water vapor in the enhanced natural gas synthesis.
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）