ACS Catalysis
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2026
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IF 13.6
Yanmei Cai,Zhirui Luo,Kok Bing Tan,Sajid Ali,Xiaoping Rao,Jian Cai,Dongren Cai,Gui-Lin Zhuang,Guowu Zhan
While conventional InNi alloy phases in supported Ni/In2O3 catalysts show limited performance for CO2-to-methanol hydrogenation, we demonstrate that carbon incorporation into the InNi3 gives rise to a distinct catalytic architecture. The saturated InNi3C0.5 exhibits better catalytic stability and 40-fold enhanced methanol productivity compared with noncarburized alloys. Although the in situ carburization of InNi3 in the CO2 hydrogenation reaction produced the unsaturated InNi3Cx, this catalyst had lower stability and activity compared to the saturated InNi3C0.5. Structural degradation mechanisms reveal atmosphere-dependent intermetallic carbon oxidation pathways in the InNi carbides. Furthermore, hierarchical engineering through an electrostatic assembly of the saturated InNi3C0.5 hexagonal nanosheets on In2O3 hollow nanotubes synergistically enhances both activity and durability. Density functional theory analysis unveils that carbon-induced electron redistribution creates Ni/C cooperation resembling uniform electron gas behavior, simultaneously optimizing hydrogenation capacity and oxygen vacancy dynamics on the oxide support. This work establishes intermetallic carbon saturation engineering as a general strategy for upgrading intermetallic catalysts in renewable fuel synthesis.
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ACS Applied Materials & Interfaces
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2026
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IF 7.8
Yanan Jiang,Yuzhen Fang,Yitian Fu,Runze Xue,Abdul Wahab,Yuan Liu,Cuijuan Zhang
ZrO2 is an effective support for CO2 methanation, but its low surface area limits the dispersion and thus activity and stability of the Ni/ZrO2 catalyst. Herein, a ZrO2/SiO2 support was constructed by dispersing nano-ZrO2 on high-surface-area SiO2 to improve the activity and anti-sintering capability of the Ni catalysts. The results showed that SiO2 stabilized the nano-ZrO2, which further provided favorable sites for dispersing and stabilizing Ni species. Ni/0.4ZS exhibited decent performance among the Ni/xZS catalysts (x was the mass ratio of ZrO2 to SiO2) due to the increased dispersion of Ni. Moderate CeO2 promoter addition further improved the activity and resistance to deactivation due to the increased dispersion of Ni NPs and the enhanced adsorption of CO2. XPS and DFT results indicated that the composite support strengthened the electronic interaction between Ni species and the support. Furthermore, based on the experimental and DFT results, it is proposed that additional geometric stabilization of Ni species may be provided by the spatially constrained sites between adjacent nano-ZrO2 particles. These findings demonstrated that constructing nano-ZrO2 on SiO2 was an effective strategy for developing active and stable Ni-based catalysts for CO2 methanation.
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CHINESE JOURNAL OF CATALYSIS
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2026
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IF 17.2
Xiaoqian Wang,Feifan Zhao,Wantian Mei,Jianjun Zhang,Chuanbiao Bie,Jiaguo Yu,Hermenegildo Garcia,Feiyan Xu
Efficient S-scheme photocatalysis requires not only favorable band alignment but also sufficiently strong interfacial driving forces to direct photogenerated carrier migration across the junction. Local donor-acceptor (D-A) coordination and global Fermi-level equilibration are shown to cooperate in the dark to precondition interfacial energetics and thereby promote subsequent S-scheme charge transfer. A molecularly coupled heterojunction is constructed by integrating a triazine-imine covalent organic framework (TPT-COF) with ZnO quantum dots through interfacial Zn–N coordination. Spectroscopic analyses reveal that D-A-induced local electron redistribution and Fermi-level-equilibration-driven compensating charge redistribution coexist in the dark, cooperatively enlarging the effective interfacial energy offset and reinforcing the internal electric field prior to illumination. Ultrafast spectroscopy further shows that this preconditioned interface accelerates S-scheme charge transfer under light irradiation, enabling efficient spatial charge separation while preserving strong redox potentials. As a result, the optimized COF/ZnO heterojunction achieves selective CO 2 photoreduction to CH 4 without external photosensitizers or sacrificial agents. These findings identify a cooperative mechanism by which local coordination chemistry and interfacial electrostatics jointly regulate S-scheme energetics, offering a molecular strategy for designing adaptive photocatalytic interfaces for solar fuel production.
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Chem Catalysis
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2026
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IF 10.7
Yulong Zhang,Zhonghao Chen,Yajing Zhang,Wenhui Sun,Wangyin Wang,Xupeng Cao,Xin Guo,Can Li
Microbial electrosynthesis can convert CO 2 into useful chemicals, but electron transport across the cell envelope remains a major limitation. Here, we introduce periplasmic gold nanoparticles (AuNPs) in Ralstonia eutropha to facilitate transmembrane electron transfer during CO 2 conversion. The AuNPs reduce interfacial charge-transfer resistance by more than 95%, enabling more efficient delivery of electrode-derived electrons into cellular metabolism. As a result, the biohybrid system shows markedly improved CO 2 reduction performance. Product selectivity can be tuned through bioelectrode design: drop-casted electrodes favor acetate production, whereas self-assembled biofilms achieve over 90% selectivity for C 4 products, with a maximum Faradaic efficiency of 44.4%, reaching 71% of the theoretical limit for aerobic CO 2 fixation. Spectroscopic, electrochemical, and transcriptomic analyses support enhanced electron transfer and carbon metabolism. This work provides a practical strategy for wiring non-electrogenic microbes and improving microbial CO 2 conversion to multi-carbon chemicals.
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AICHE JOURNAL
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2025
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IF 4
Meili Ding,Wei Rong,Yang Wang,Jianfeng Yao
Reforming desirable photocatalytic platforms for efficient carbon dioxide (CO 2 ) utilization is highly desirable but represents a great challenge. In this study, we report a facile surface structure modulation strategy to fabricate functional biochars (BCs) with different surface oxygen functional groups. The mild oxidation of sodium hypochlorite endows BC with abundant surface oxygen species without significantly compromising its inherent morphology. Under Xe lamp irradiation (400 mW/cm 2 ) and 1 bar CO 2 , the catalytic activity toward the coupling of CO 2 and epichlorohydrin based on BC-NaClO reached 100% yield, which was 3.8, 2.6, and 1.5 times greater than that of pristine BC, functional BC-HNO 3 , and BC-NaOH, respectively. Further investigations revealed the contributions of both holes and electrons to the photocatalytic activity of BC-NaClO and the synergistic effects of photocatalysis and photothermal catalysis. This work demonstrates a rational pathway toward high-efficiency biomass-derived photocatalysts for targeted CO 2 conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Hui Kang,Chen-Ning Li,Lifei Yin,Jiabao Gui,Meng Wang,Yang Chen,Jinping Li,Libo Li
The separation of carbon dioxide (CO 2 ) from acetylene (C 2 H 2 ) is crucial but highly challenging due to their similar molecular dimensions and physicochemical properties. In contrast to C 2 H 2 -selective adsorbents, CO 2 -selective adsorption strategy substantially reduces energy consumption by eliminating the need for additional C 2 H 2 desorption steps. However, the development of CO 2 -selective adsorbents capable of reversing C 2 H 2 /CO 2 separation remains limited and requires further exploration. Herein, we report a porous coordination polymer, [Cu(5-NH 2 -ipa)(pia)], featuring an interdigitated structure with one-dimensional corrugated channels to directly purify C 2 H 2 . Adsorption results indicate that at 298 K and 1.0 bar, [Cu(5-NH 2 -ipa)(pia)] exhibits a CO 2 /C 2 H 2 uptake ratio of 2.09 and IAST (Ideal adsorbed solution theory) selectivity of 10.9. It possesses optimally sized pores with an electrostatic potential that is highly complementary to the electrostatic properties of CO 2 , enabling preferential CO 2 adsorption through strong electrostatic interactions and hydrogen bonding. This result is well supported by molecular simulation and theoretical calculations. Furthermore, experimental breakthrough tests demonstrate that high-purity CO 2 can be directly obtained from CO 2 and C 2 H 2 mixtures. This work paves the way for the future development of advanced porous materials and inspires their use for CO 2 -selective capture from C 2 H 2 .
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PubMed
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Journal of CO2 Utilization
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2025
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IF 8.4
Kihyuk Sung,Hye Jeong Joe,Changsu Ha,Hee-Seong Yang,In-Hwan Lee,Seok Ki Kim,Hye-Young Jang
We investigated the polymerization mechanism of a highly active heterogeneous Zn-gallate catalyst used for propylene oxide (PO) homopolymerization and PO/CO 2 copolymerization. The molecular weights of poly(propylene oxide) (PPO) and poly(propylene carbonate) (PPC) can be controlled by varying the ratio of chain transfer agents (CTAs) to PO. CTAs of varying acidity and structure provided insight into their interaction with catalytic sites. Theoretical calculations on a heterogeneous zinc hydroxide slab model for Zn-gallate revealed that polymerization is initiated by the reaction of PO with a hydroxyl group located within the zinc hydroxide lattice. Further energy barrier calculations and polymerizations at varying CO 2 pressures explained the kinetic preference for PPC formation over PPO at high CO 2 pressure.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Tianyi Wang,Longqi Wu,Chao Zhang,Guozhu Zhang,Yang Chen,Chengze Gao,Zeyu Wang,Yiming Wang,Yang Gao,Fuzhen Xuan
Real-time monitoring of exhaled carbon dioxide (CO 2 ) is essential for assessing metabolic status and tracking disease progression. However, the high moisture content of exhaled breath poses a significant challenge to the accuracy and stability of CO 2 detection. Here, we present a flexible chemiresistive CO 2 sensor based on a dimethylamine-functionalized hydrogel, in which water molecules critically facilitate the CO 2 -induced reversible protonation of tertiary amine groups, thereby modulating the hydrogel's ionic conductivity for real-time breath analysis. As a result, the hydrogel synthesized from N -[3-(dimethylamino) propyl] methacrylamide (DMAPMA) exhibits a high CO 2 response of 37.3 % at 10,000 ppm and a low detection limit of 100 ppm. To further enhance mechanical durability under respiratory-induced stress, N , N -Dimethylacrylamide (DMAA) was incorporated into the hydrogel, increasing the tensile strain limit from 34.2 % to 51.0 % without compromising CO 2 sensing performance. In addition, we demonstrate the integration of the hydrogel sensor into a wireless smart mask system, enabling multimodal monitoring of respiratory CO 2 patterns, physical activity, and postprandial metabolic changes. This platform offers a scalable, low-power solution for wearable CO 2 sensing in personalized health monitoring.
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Journal of CO2 Utilization
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2025
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IF 8.4
Dake Zhang,Wenzhen Wang,Zhen Wang,Dengmeng Song,Shuang Liu,Yuyang Chen,Xiaoni Ma,Li Xia
Addressing the challenges of biotoxicity, poor long-term stability, and inadequate interfacial adhesion that hinder the clinical translation of tissue adhesives, we utilized the biocompatibility and biodegradability of CO₂-derived polycarbonates (PPC) and innovatively incorporated diacetyl-L-tartaric anhydride (DATA) into the copolymerization to develop PPC and DATA alternating/random copolymer (PPCD) bioadhesives. Compared to unmodified PPC, PPCD exhibits significantly enhanced adhesive properties: peel strength increased to 4.7 ± 0.43 N/cm (a 273 % improvement), sealing strength reached 67 ± 2.3 kPa (a 235 % enhancement), and skin adhesion strength rose to 22.1 ± 2.3 kPa (a 203 % increase). In comparative tests, PPCD outperformed commercial Fibrin glue in overall mechanical performance. Furthermore, PPCD demonstrates thermoresponsive viscosity modulation, undergoing debonding at 10°C with a thermal response efficiency exceeding 95 % compared to its viscosity at 37°C. Crucially, PPCD retains the degradability and bioaffinity of the original PPC, as confirmed by cytotoxicity assays showing > 98 % cell viability and histopathological analyses in mice verifying its biosafety. This bioadhesive resolves the long-standing trade-off between mechanical robustness and biocompatibility, while also establishing a new CO₂ valorization strategy for eco-friendly biomedical materials. The functionalization of PPC not only enhances adhesive performance but also pioneers a sustainable pathway for carbon utilization, demonstrating the transformative potential of next-generation tissue repair technologies.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Zhilv Chen,Chaoming Jian,Chao Li,Tao Wang,Qinhui Wang,Mengxiang Fang,Fanpeng Meng,Wei Chen,Yongsheng An,Ximing Hu
Traditional aqueous amine-based absorbents face high energy consumption challenges in CO₂ capture processes. Replacing water with organic solvents of low viscosity, low specific heat, and high boiling point in amine-based CO₂ absorbents can effectively reduce the sensible and latent heat required for solvent regeneration. However, the introduction of organic solvents significantly alters mass transfer kinetics and chemical equilibrium, and the quantitative relationship between these effects remains unclear. In this study, water-lean absorbents EFH series with varying organic solvent concentrations were formulated using N , N -dimethyl-1,2-ethanediamine(DMEDA), N , N -dimethylformamide (DMF), and water. Kinetic parameters were measured for DMEDA aqueous solutions, MEA aqueous solutions, pure DMF, and the EFH series. The results revealed an inconsistency between the liquid film mass transfer coefficient ( kₗ ) and viscosity trends, indicating that physical mass transfer dominates the efficiency limitation of DMEDA absorbents under low CO₂ loading, while DMEDA retains sufficiently rapid chemical reaction rates even in water-lean environments. 13 C NMR analysis demonstrated that carbamate species exist as incompletely dissociated ion pairs in aprotic solvent environments. The stabilization of these ion pairs by organic solvents suppresses the generation of neutral carbamic acid, thereby restricting mass transfer and leading to an inflection point in the absorption rate. These findings highlight a dual strategy for optimizing water-lean absorbents: (1) prioritizing low-viscosity, high-CO₂-solubility solvents to enhance initial mass transfer, and (2) tuning solvent polarity or introducing proton donors to sustain reaction efficiency at higher CO₂ loadings. This work provides quantitative mechanistic insights into balancing the trade-off between chemical equilibrium and mass transfer in non-aqueous systems, offering guidance for designing energy-efficient carbon capture solvents.
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ACS Applied Nano Materials
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2026
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IF 5.8
Meidan Que,Xiangwei Bai,Tengjiao Xue,Ziang Liu,Jiaojiao Zheng,Xun Sun,Jun Xu
Barium titanate (BaTiO3) exhibits high chemical stability; however, the relatively rapid recombination of charge carriers severely limits its photocatalytic performance. Meanwhile, electrocatalysis facilitates charge transport by generating a spontaneously polarized electric field, effectively suppressing charge carrier recombination, but the performance of conventional ferroelectric catalysts is inherently constrained by their low surface piezopotential. In this study, a piezo-photocatalytic system triggered by ultrasonic vibration is reported, based on BaTiO3 nanobats. The BaTiO3 structure resembles a nanobat, featuring a thicker lower cylindrical body (∼35 nm diameter) and a thinner upper section (∼20 nm diameter) with a total length of about 250 nm. It can generate a piezo-potential as high as 1.2 V through COMSOL finite element simulation. Under mild vibration, the BaTiO3 nanobats exhibit superior piezo-photocatalytic performance, converting CO2 into CO with a maximum yield of 101.18 μmol·g–1·h–1. The yield is approximately five times higher than that achieved with ultraviolet light irradiation alone. Furthermore, theoretical calculations reveal that the adsorption and desorption of intermediates (*COOH, *CO) on BaTiO3 can be regulated by applying different strains. The piezo-photocatalytic CO2 reduction reaction opens an avenue beyond conventional photocatalysis, expanding energy utilization to pave the way for carbon neutrality.
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ACS Catalysis
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2026
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IF 13.6
Tingting Ge,Runhua Chen,Xiaorui Liu,Ziyan Jia,Chao Liu,Jiahui Huang,Yongfu Sun
Electrocatalytic reduction of CO2 to methane is one of the effective strategies for achieving carbon cycling and addressing environmental issues. Herein, we report the successful synthesis of an atomically precise Cu58 nanocluster. An optimized one-pot method involving sequential sodium borohydride reduction was developed. The crystal structure of the Cu58 nanocluster belongs to the space group Pca21 and features a central distorted face-centered cubic Cu14 kernel encapsulated within a Cu48S36P4 shell. This shell is composed of Cu7S2 and Cu10S8P2 units and is flanked by two peripheral Cu5S5P staple motifs. ESI-MS confirms the molecular formula, and XPS analyses establish that copper exists exclusively in the Cu+ oxidation state. The catalytic performance of Cu58 was evaluated for electrochemical CO2 reduction (CO2RR) upon dispersion on a C3N4 support. 15-Cu58/C3N4 achieves a CH4 Faradaic efficiency of 73% at 600 mA cm–2. The synergy between the topology structure of Cu58, the Cu+ sites of the nanocluster, and the pyridinic N sites of the C3N4 support is identified as the key factor for enhancing CO2 adsorption and suppressing the competing hydrogen evolution reaction, thereby steering the selectivity toward methane. This study underscores the potential of structurally defined copper nanoclusters as the premier electrocatalysts for fuel production.
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