CHEMICAL ENGINEERING SCIENCE
·
2026
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IF 5.1
Hanlin Wang,Xianglin Chen,Yafei Guo,Pu Huang,Antian Wang,Jingyi Shi,Huaxiang Gao,Ruilin Wang,Chuanwen Zhao
Electrochemical CO 2 reduction to syngas driven by renewable energy offers a sustainable alternative to conventional fossil-fuel-based processes, while maintaining a stable H 2 /CO ratio under the inherently fluctuating potentials remains a substantial challenge. In this study, a series of supported Zn catalysts are fabricated by electrodepositing Zn onto Cu foil substrates, with a systematic investigation into the effects of deposition current density (−5 to −20 mA/cm 2 ) and deposition time (10 to 20 min) on catalyst structure and performance. Characterization results reveal that, with increasing deposition parameters, Zn species evolve from discrete nanoplates into an interwoven network of wrinkled structures, accompanied by decreased work function and charge transfer resistance. The synthesized catalysts exhibit a favorable balance in activity toward the electrochemical CO 2 reduction reaction (eCO 2 RR) and hydrogen evolution reaction (HER), thereby enabling highly tunable syngas production with H 2 /CO ratios ranging from 0.5 to 5.4. Notably, the Cu-Zn catalysts demonstrate remarkable stability in syngas composition, maintaining a nearly constant H 2 /CO ratio across a wide potential window of −1.11 to −1.41 V vs. reversible hydrogen electrode (RHE). Furthermore, the Cu-Zn-10–10 catalyst exhibits excellent durability under fluctuating voltage conditions over 24 h, highlighting its potential for seamless integration with intermittent green electricity. In-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations indicate that the Cu-Zn bimetallic sites moderately enhance *CO adsorption, inhibiting its rapid desorption. Moreover, the energy barriers of eCO 2 RR and HER show little variation with potential, which collectively ensure the stability of the H 2 /CO ratio within the range of −1.11 to −1.41 V vs. RHE.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Xiaoyang Xu,Yong Zhang,Qiliang Wu,Fenghai Cao,Hua Yang,Diwen Zhou,Yang Chen,Thachapan Atchimarungsri,Lizhi Wu,Chen Yang,Sen Wang,Li Tan
Two Cu/Mo 2 C catalysts with different interfacial structures are synthesized to reveal how synthesis routes control CO 2 hydrogenation selectivity. • 5Cu/Mo 2 C‑IWI achieves 85.7% methanol selectivity and STY of 53.7 mg MeOH ·g cat −1 ·h −1 , outperforming its doped counterpart that predominantly yields CO and CH 4 . • Moderate metal‑support interaction over catalyst stabilizes Cu δ+ /Mo 6+ for CO 2 conversion to methanol. • In situ DRIFTS verified catalysts follow dual formate-carboxylate pathway, and Cu/Mo 2 C interfacial structure regulates intermediates evolution to determine final product distribution. The conversion of carbon dioxide (CO 2 ) into methanol using renewable energy has dual energy and environmental significance. Molybdenum carbide (Mo 2 C) exhibits excellent CO 2 activation ability and thermal stability, but it is still difficult to achieve high methanol selectivity for catalysts supported on it, and the structure-activity relationship between interface structure and selectivity is still unclear. Here, Cu/Mo 2 C-IWI and Cu@Mo 2 C catalysts were fabricated via incipient wetness impregnation and in situ doping strategies, respectively, to investigate the effect of different Cu/Mo 2 C interfaces on product selectivity. Among them, Cu/Mo 2 C-IWI exhibited high methanol selectivity of 85.7% with a space-time yield of 53.7 mg MeOH ·g cat −1 ·h −1 (230 ℃, 3 MPa), whereas Cu@Mo 2 C predominantly produced CH 4 and CO. Combined X-ray photoelectron spectroscopy and Auger electron spectroscopy results revealed that moderate metal-support interactions in Cu/Mo 2 C-IWI stabilized the higher valence states of Cu δ+ and Mo 6+ species, which are critical for stabilizing formate (HCOO*) and carboxylate (*COOH) intermediates. In contrast, abundant Mo 2+ species and rich oxygen vacancies on Cu@Mo 2 C facilitated the cleavage of C–O bonds, thus promoting CO and CH 4 formation. In situ diffuse reflectance infrared spectroscopy ( in situ DRIFTS) verified that both catalysts follow a dual-path reaction mechanism involving formate and carboxylate intermediates, and interfacial structure dominates the evolution of reaction intermediates and final product distribution. This study establishes a clear correlation among synthesis strategy, interfacial structure and catalytic selectivity, and demonstrates that constructing surface Cu/Mo 2 C interfaces serves as a rational design principle for highly selective hydrogenation of CO 2 to methanol. Download: Download high-res image (210KB) Download: Download full-size image
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Science China-Materials
·
2026
·Vol. 69
·期 3
·1486-1498
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IF 7.7
Wu Qiaolin,Liu Xingyu,Cheng Lei,Tang Yawen,Li Yafei,Wang Yu,Sun Hanjun
Construction of metal-mediated redox sites is an appealing approach to enhance photocatalytic CO 2 reduction coupled with H 2 O oxidation. However, conventional static redox sites generally lack spatiotemporal matching during reaction processes due to the constraints of rigid structure and the linear scaling relationship of adsorbed species. Herein, an alkanolamine-Ir synergistic system was developed, where flexible monoethanolamine (MEA) molecules function as molecular ferries to selectively adsorb CO 2 via carbamate formation, while adjacent Ir nanoparticles (NPs) serve as H spillover hubs that relay protons, creating spatiotemporal adaptability that synchronizes CO 2 reduction and water oxidation. In addition, time-resolved in situ spectroscopy directly captures the rapid transformation of carbamate intermediates concurrent with sustained IrOOH intermediates formation. Microkinetic modeling further demonstrates that the MEA-Ir modified system (M-Ir/ACN) creates interconnected H spillover networks between Ir NPs and MEA, facilitating efficient proton transport that drives *COOH formation with a favorable thermodynamic energy. As a result, the M-Ir/ACN achieves a 20-fold increase in CO production compared to the pristine sample while maintaining high stability throughout 45 h of continuous operation. This study presents that flexible molecular ferries boost CO 2 adsorption, and deciphers how flexible molecular-metal synergy directs the trafficking of CO 2 -derived intermediates toward highly efficient CO 2 photoreduction.
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BIORESOURCE TECHNOLOGY
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2026
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IF 8.2
Li Sun,Cao Zhenzhou,Cui Jixian,Huang Liuyang,Qi Xiaonan,Wei Yanjie,Li Xianhui
Developed Fe 2 O 3 NPs-embedded membranes to overcome gas–liquid mass transfer limits. • Fe 2 O 3 NPs raise surface area and add C O groups, thereby enhancing CO 2 adsorption. • Fe 2 O 3 NPs-nanofiber membranes enhance biomass, CO 2 fixation, and delay decline. • Fe 2 O 3 NPs promote stable biofilm formation, enhancing initial attachment and growth. • Fe 2 O 3 NPs enhance ATP, photosynthesis and XDLVO adhesion for CO 2 fixation performance. Algae-based carbon capture and utilization (CCU) technique offers a sustainable strategy for CO 2 mitigation, but its efficiency is often limited by poor gas–liquid mass transfer and unstable carbon availability. Here, this study developed an iron oxide nanoparticle (Fe 2 O 3 NPs)-incorporated electrospun nanofiber membrane to enhance CO 2 capture and microalgal fixation. Results revealed that the Fe 2 O 3 NPs was able to reduce fiber diameter, refine pore architecture, and increase specific surface area, thereby the improved CO 2 adsorption. In Chlorella cultivation, the final biomass concentration and CO 2 biofixation rate of modified membrane increased by respective 11.6%±1.2% and 14.3% compared with that of pristine nanofibers. Furthermore, the modified membrane significantly promoted the early-stage biofilm formation, yielding biofilms that were 47.9% thicker, denser, and exhibited increased rougher surface. Nanoparticle-induced “microhooks”, together with enhanced EPS secretion, strengthened algal attachment, increased cell density, and improved spatial homogeneity, thus creating a favorable microenvironment for rapid biofilm development. Cellular analyses demonstrated that membranes modified with Fe 2 O 3 NPs increased intracellular ATP by 45.6%, superoxide dismutase activity by 39.9%, and specific growth rate by 41.8% compared to the blank controls, indicating enhanced metabolic activity and stress resistance. Physicochemical characterization further showed that a reduction in electrostatic repulsion and an increase in hydrophobicity. Meanwhile, Lifshitz-van der Waals (U LW ) and Lewis acid-base (U AB ) interaction energies increased by approximately twofold and 2.74-fold, respectively. These changes synergistically enhanced initial algal adhesion and attachment stability, facilitating CO 2 enrichment. In summary, this work elucidates the synergistic bio-physicochemical mechanisms underlying nanoparticle-modified membranes and specify their potential for advancing efficient microalgae-based CCUS technologies. Download: Download high-res image (191KB) Download: Download full-size image
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Chen Chi,Xue-Lu Chen,Jian Li,Jin Li,Xing-Hua Xia
Plasmonic nanostructures can utilize solar energy to drive the CO2 conversion. However, noble metals such as gold and silver struggle to mediate multielectron reduction pathways to value-added products. Here, a spatially separated plasmonic–semiconductor hybrid catalyst is designed by coupling MoS2 quantum dots to Au triangle nanoprisms. This hybrid enables hot electrons generated from both interband and intraband transitions in Au to cross over the Au–MoS2 interfacial barrier and inject into MoS2, thereby improving both the selectivity and activity of the electrocatalytic CO2 reduction reaction (CO2RR). The interband hot electrons with energies near the Au Fermi level tend to correlate with the formation of C1 products, selectively enhancing methanol production at low overpotential and promoting formic acid at higher overpotentials; meanwhile, the high-energy intraband hot electrons consistently associate with C–C coupling, significantly increasing ethanol selectivity. These results highlight the unique advantage of spatially separated catalysts in plasmon-mediated electrochemical reactions, providing an approach to utilize interband/intraband hot electrons for efficient and selective CO2RR.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Delin Yin,Lei Chen,Junmei Chen,Jin Yuan,Jianguo Liu,Xin Kong
Perfluorooctanoic acid (PFOA) is a persistent emerging contaminant that has attracted increasing attention due to its recalcitrance and toxicity. This study demonstrates the efficacy of a zero-valent iron (Fe 0 ) mediated biogas upgrading system for simultaneous PFOA degradation and methane production, with PET microplastics playing a secondary role in the degradation process. At a PFOA dosage of 0.3 mg/L, defluorination efficiencies ranging from 21.22% to 31.98% were achieved after five biogas upgrading cycles (approximately 25 days), accompanied by enhanced CO 2 methanation performance (ultimate CH 4 content >95%). At a PFOA concentration of 10 mg/L, analysis of extracellular polymeric substances (EPS) revealed a significant decrease in protein content within the reactors. Molecular docking models and reactive oxygen species (ROS) analyses suggested that the binding of PFOA to specific amino acid residues mitigated its cytotoxicity. The microbial community in the Fe 0 -mediated reactor was dominated by Methanosaeta , a strictly acetoclastic methanogen. Furthermore, metagenomic analysis indicated the upregulation of key genes associated with methanogenesis and fluoride transport under Fe 0 mediation. Characterization of infrared spectrum and fluorinated metabolic intermediates suggested that PFOA degradation proceeded primarily via stepwise decarboxylation pathways. This study not only confirms the roles of Fe 0 and PET microplastics in PFOA removal but also reveals the synergistic metabolic coupling between defluorination and methanogenesis, therby elucidating the mechanisms of Fe 0 -enhanced PFOA degradation.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2026
·
IF 4.8
Youwei Wu,Ning Zhou,Tingyan Peng,Weixin Ma,Lili Qiu,Fei Xue,Zhifeng Dai,Yubing Xiong
Poly(ionic liquids) (PILs) offer many inherent advantages in material design, owing to their tunable structure, polarity, and versatile functionalization capability. These properties make PILs highly promising candidates for heterogeneous catalysis, especially carbon dioxide (CO 2 ) conversion and utilization. In this work, a triazine-functionalized isocyanate monomer and an amino-functionalized imidazolium-based PIL were designed and synthesized. Through the addition polymerization, a family of novel urea- and triazine-functionalized porous PIL heterogeneous catalysts (denoted as p-PIL-x) were prepared. The resulting materials were thoroughly characterized by Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and CO 2 adsorption measurements. The catalysis evaluation revealed that p-PIL-x promotes efficient CO 2 conversion via intramolecular synergy among the urea, triazine, and imidazole motifs, all of which are rich in nitrogen species. Under optimized conditions (0.1 MPa, 80 °C, 24 h), the catalyst achieved a cyclic carbonate yield of 94.33% with 99% selectivity. The reaction mechanism was further elucidated through density functional theory (DFT) calculations and in situ FT-IR measurement, which highlighted the cooperative role of hydrogen-bond donors and bromide ions in activating both the epoxide substrate and CO 2 . The synthesized p-PIL-x catalyst exhibits excellent heterogeneity, stability, and recyclability, offering a promising platform for the development of multifunctional heterogeneous catalysts toward efficient and sustainable CO 2 conversion.
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高影响因子
ACS Omega
·
2026
·
IF 5.2
Jiaozhu Wu,Jiaxi Zhang,Xutao Zhang,Haoyu Ma,Jie He,Qiang Liu,Guangxian Li,Pengjian Gong
Abstract The microwave absorption performance depends on both impedance matching and electromagnetic energy dissipation. Conventional filler-functionalized polyimide (PI) composites can provide strong electromagnetic attenuation, but their limited foamability under supercritical carbon dioxide (scCO2) restricts porous structure formation and thus impairs impedance matching. To address these limitations, this study proposes an intrinsic molecular modification strategy based on a chain segment design. Furthermore, by combining synergistic dielectric-magnetic loss from nanofillers with a double-layer heterogeneous architecture, a PI-based electromagnetic shielding nanocomposite with strong microwave absorption performance and low-reflection characteristics was constructed. Bisphenol A dianhydride (BPADA) was used as the dianhydride monomer, and a series of PI copolymers with tunable chain segment compositions were prepared through the reaction of BPADA with mixed aromatic diisocyanate (MDI) and aliphatic diisocyanate (HDI), followed by thermal imidization/cyclization. The changes in molecular chain mobility, scCO2 foaming behavior, and cellular structure associated with the nominal HDI feed fraction were systematically investigated. The results showed that increasing the nominal HDI feed fraction was associated with an improved rigid-flexible balance of the PI backbone, enhanced segmental mobility, a broader foaming window, and the formation of PI foams with uniform and compact cellular structures. CNT@Fe3O4 nanofillers with both dielectric and magnetic loss capabilities were further introduced to improve the intrinsic electromagnetic loss of the composite foams. The calculated microwave absorption results showed that, after pore structure regulation, the PI/CNT@Fe3O4 nanocomposite foam exhibited markedly enhanced microwave absorption in the X-band. At a porosity of 46 vol %, the minimum reflection loss reached −38 dB at a thickness of 2 mm. A double-layer heterogeneous structure comprising a CNT@Fe3O4-containing porous absorbing layer and a CNT-containing dense reflecting layer was then constructed to exploit impedance gradient transition, dielectric-magnetic synergistic loss, and multiple reflection/reabsorption processes. The optimized sample showed an average absorption coefficient of 0.92 in the X-band and a maximum A/R ratio of 332, indicating pronounced high absorption and low reflection characteristics. This study provides a new strategy for designing and fabricating lightweight, high-performance PI-based electromagnetic protection materials with an absorption-dominated shielding behavior.
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高影响因子
ACS Applied Polymer Materials
·
2026
·
IF 5.2
Yuqi Sun,Ziliang Wang,Xue Wang,Yutong Liu,Baixue Li,Yusheng Qin
Abstract CO2-based polycarbonates represent an important class of sustainable polymers derived from carbon dioxide utilization. However, the inherent absence of functional groups hinders the use of these materials in high-value applications. To address this challenge, we combined click chemistry with the Kabachnik–Fields reaction for sequential postpolymerization modification of CO2-based polycarbonates. This strategy not only introduced biobased multifunctional pendants along the polycarbonate backbone but also enhanced the mechanical strength, thermal stability, flame retardancy, and hydrophilicity of the resulting films. Notably, the incorporation of α-aminophosphonate via the Kabachnik–Fields reaction imparted the resulting polymers with unconventional fluorescence and typical aggregation-induced emission (AIE) characteristics. This work provides a general and robust strategy for the rational design of functional aliphatic polycarbonates toward practical applications.
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高影响因子
ACS Applied Energy Materials
·
2026
·
IF 5.5
Fuwei Sun,Yao Li,Ziang Huang,Weigang Liu,Chao Liu,Rui Wang,Pengcheng Li,Chen Wang,Bo-Qing Xu,Guangtao Li
Abstract Au/TiO2 is a promising photocatalyst for CO2 reduction, yet its performance is often limited by inefficient light utilization and insufficient local CO2 availability. Here, we present an integrated photocatalytic platform by embedding Au/TiO2 nanoparticles within imidazolium poly(ionic liquid) (PIL) nanocone arrays. The nanocone architecture provides broadband light harvesting with > 99% absorptivity, while the imidazolium PIL enriches CO2 near the catalytic sites, enabling synergistic enhancement of CO2 photoreduction. The intrinsic counter-anion exchangeability of the PIL further enables programmable regulation of the overall catalytic activity and product formation selectivity. By optimizing the counter anion and water supply, the system selectively produces CO (124.89 μmol·g–1·h–1, 94.2% selectivity) or CH4 (137.75 μmol·g–1·h–1, 100% selectivity). Metalloporphyrin counter anions additionally enable C2 product formation, while functional catalytic anions allow cascade conversion of CO2 into polymeric products. This work demonstrates an integrated strategy that couples light management, substrate enrichment, and reaction programmability for efficient and versatile solar-driven CO2 conversion.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Mei Yang,Jingtian Yang,Ruobing Pi,Pingtao Fang
Corn-straw-derived CQDs are prepared via a hydrothermal method. • CN/NC/CQDs-6 achieves a CO evolution rate of 37.37 μmol g −1 h −1 . • CQDs improve charge separation and facilitate interfacial charge transport. Photocatalytic CO 2 reduction is a promising approach for mitigating energy shortages and carbon emissions. Herein, graphitic carbon nitride (g-C 3 N 4 ) was employed as the substrate and combined with hydrothermally synthesized NiCo-LDH, followed by the introduction of carbon quantum dots (CQDs) to fabricate a series of CN/NC/CQDs-x ternary composites. The composite exhibited enhanced absorption in the visible spectral region and improved photoinduced charge-separation behavior. Meanwhile, the integration of NiCo-LDH, g-C 3 N 4 , and CQDs promoted interfacial coupling, suppressed the recombination of photogenerated carriers, and facilitated charge separation and transport within the ternary composite. In addition, the CO 2 photoreduction activity of CN/NC/CQDs-x composites was evaluated. Among the prepared samples, CN/NC/CQDs-6 shows the best photocatalytic performance, achieving a CO generation rate of 37.37 μmol g −1 h −1 , which is 26.31 times that of pristine g-C 3 N 4 . This work provides insights into the development of biomass-derived CQD-modified g-C 3 N 4 photocatalysts for efficient CO 2 reduction.
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高影响因子
SusMat
·
2026
·
IF 19.2
Yongzheng Gao,Xin Tao,Yanli Chen,Xinqian Yu,Yijun Zhu,Yongchao Liang,Qiong Peng,Xiu Gong,Xiaosi Qi,Guangmin Zhou
Spinel oxides have attracted increasing attention as cathode in Li–CO 2 batteries because of their cost–effectiveness and facile synthesis. Unfortunately, their catalytic activity for CO 2 reduction reaction and CO 2 evolution reaction remains below the necessary for the implementation at scale. Here, the introduction of first–row 3d transition metals (TMs) in Fe 3 O 4 can construct an asymmetric M–O–Fe backbone, which is defined as the bond strength polarization and leads to continuous modulation in the electron activity (TM used in this work including Mn, Co, Ni, and Cu). Theoretical calculations confirm that the bond strength polarization can optimize the adsorption behavior of the reactants (CO 2 , Li + , and Li 2 CO 3 ), promoting the catalytic activity toward CO 2 reduction and CO 2 evolution. Experimental and theoretical results display a volcano–shaped relationship between the bond strength polarization and the catalytic activity in the TM–doped Fe 3 O 4 cathodes. The decisive role of the discharge product morphology in battery performance is also delineated. These findings enable the design of an efficient catalyst, Mn–Fe 3 O 4 , which can run stably up to 2000 h with a low voltage gap of ∼0.8 V. This work offers a rational viewpoint for tuning the catalytic activities of TM oxides in Li–CO 2 batteries.
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高影响因子
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