ACS Catalysis
·
2026
·Vol. 16
·期 17
·17380-17391
·
IF 13.6
Ma Meifeng,Zhang Rongwang,Deng Shaorong,Zhao Xilai,Yang Fei,Fang Xiuzhong,Wang Xiang,Xu Xianglan
Rational design of highly active catalysts for low-temperature CO 2 methanation remains a critical challenge for efficient CO 2 utilization. Herein, we demonstrate that Mn incorporation into the Cr 2 O 3 lattice, rather than surface modification, markedly enhances the catalytic performance of Ru/Cr 2 O 3 catalysts. The optimal Ru/Mn 0.10 Cr 0.90 O x catalyst (2.24 wt % Ru) achieves 91% CO 2 conversion at 200 ° C with a space velocity of 36,000 mL g cat –1 h –1 , substantially exceeding that of the parent Ru/Cr 2 O 3 (4% at 200 ° C). Compared with Ru/Cr 2 O 3 , Ru/Mn 0.10 Cr 0.90 O x exhibits a 4.1-fold higher turnover frequency at 180 ° C, confirming the intrinsic catalytic enhancement conferred by Mn lattice doping. Comprehensive characterization revealed that Mn lattice doping generates Mn-O-Cr bonds, creating distinct Ru/O-Cr-O v -Mn interfacial sites in contrast to the Ru/O-Cr-O v -Cr interfaces present in undoped Ru/Cr 2 O 3 . In situ DRIFTS and H 2 -TPSR-MS studies demonstrated that low-temperature CO 2 methanation on Ru/Mn 0.10 Cr 0.90 O x proceeds concurrently via both CO* and HCOO* intermediate pathways, whereas only the CO* pathway operates on Ru/Cr 2 O 3 . DFT calculations revealed that Mn doping selectively modulates CO 2 adsorption at the interface while minimally affecting bridged Ru sites. At the Ru/O-Cr-O v -Mn interface, oxygen vacancies form and regenerate more readily than at the Ru/O-Cr-O v -Cr interface during CO 2 methanation, enabling an additional HCOO* pathway. This dual-pathway mechanism fundamentally underpins the enhanced low-temperature activity of Ru/Mn 0.10 Cr 0.90 O x and provides a promising design strategy for developing efficient CO 2 methanation catalysts.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2026
·
IF 7.1
Wenzheng Hou,Duoyong Zhang,Jiarui Ji,Xinnan Cui,Huashan Bao,Chen Zhang,Liwei Wang
Polymer-mediated strategy enables AlFum with regulated pore structure. • Microporous domains are enhanced while the AlFum framework remains intact. • The optimized AlFum achieves a 25.5% higher CO 2 uptake at 0.15 bar. • Sorption heat of the materials remains far below typical amine-loaded sorbents. The compact crystallization and dense particle aggregation of aluminium fumarate (AlFum) may limit the effective utilization of its intrinsic microporous sorption domains for CO 2 capture. To address these limitations, a pore-structure regulation strategy is developed by employing polyethyleneimine as a transient polymeric modulator during the synthesis of AlFum. Unlike conventional amine-loading strategies that enhance CO 2 affinity through retained amine-rich phases but may sacrifice microporosity and increase sorption energetics, this approach is associated with dosage-dependent changes in particle assembly and textural pore development while preserving the intrinsic AlFum framework. The optimized AlFum(PEI-0.2) delivers the best CO 2 sorption performance among the series, with a 25.5% uptake enhancement at 0.15 bar. Despite the improved capacity, it maintains a moderate isosteric heat of 21–25 kJ mol −1 , consistent with predominantly physisorption-based and reversible CO 2 sorption. Delayed CO 2 breakthrough and increased dynamic CO 2 uptake under 15% CO 2 /85% N 2 demonstrate enhanced dynamic CO 2 retention for AlFum(PEI-0.2), while five consecutive breakthrough cycles at 30% RH retain 96.6% of the first-cycle uptake. GCMC simulations further identify the intrinsic micropores of ideal AlFum as preferential equilibrium CO 2 sorption domains. This strategy establishes a pore-structure design enabled by transient polymeric modulation, balancing intrinsic microporous domains with textural pore development and providing a promising route toward stable Al-based MOF adsorbents for CO 2 capture. Download: Download high-res image (213KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Faisal Irshad,Dan Zhang,Hamzah A.S.M. Yaseen,Xianming Zhu,Muhammad Chawla,Shengping Wang,Yongli Shen,Xinbin Ma
Pd/H-MOR exhibits superior catalytic activity and stability for CO 2 hydrogenation to formateover other Pd/Zeolites and M/H-MOR. • Brønsted acid sites at Pd-H-MOR interface polarize CO 2 , while highly dispersed Pd nanoparticles dissociate H 2 barrierlessly. • Low Si/Al ratio optimizes metal-support synergy and reducing apparent activation energy to HCOOH. • Bicarbonate identified as the key reaction intermediates by in-situ DRIFTS and DFT study. Catalytic hydrogenation is a promising route for CO 2 conversion, yet the highly efficient formation of formic acid remains challenging. Herein, Pd nanoparticles dispersed on mordenite (Pd/H-MOR) are reported as an efficient and stable catalyst for CO 2 hydrogenation to produce formates. Under optimized conditions, Pd/H-MOR achieved an intrinsic turnover number of 1828 and a turnover frequency of 914 h −1 at 120 °C, surpassing all the other prepared catalysts with different metal active sites and zeolite supports. The high activity arises from the co-effect of Pd and the H-MOR support: Pd sites dissociate H 2 into active hydrogen, while Brønsted acid sites enhance CO 2 adsorption via polarization and stabilize bicarbonate intermediates, which subsequently convert to formates. Density functional theory (DFT) results revealed that Pd/H-MOR lowers the activation barriers for both H 2 dissociation and CO 2 activation at the Pd-MOR interface and combined with in-situ DRIFTS, identifying surface bicarbonates as the key reactive intermediates en-route to formate formation. Comparatively, kinetic studies of Pd/H-MOR revealed a reduced apparent activation energy of 15.81 ± 0.79 kJmol −1 , reflecting strong metal-support interactions, while the observed R = k ∙ P CO 2 0.56 ∙ P H 2 0.62 reaction orders indicate that the reaction rate is weakly dependent of H 2 and CO 2 pressures but strongly dependent on the nature of the metal and the zeolite support. This work highlights metal dispersion and support acidity as key factors for CO 2 hydrogenation. Download: Download high-res image (224KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Zhang Shaowei,Wang Shuo,Liu Hewei,Zou Geng,Guo Yige,Zhang Wenwen,Yu Lina,Liu Haolin,Zhang Xiaomin,Li Mingrun,Zhang Peng,Yu Runsheng,Zheng Xusheng,Song Yuefeng,Wang Guoxiong,Bao Xinhe
Single-atom catalysts (SACs) offer high atomic efficiency and catalytic activity but are prone to aggregation and degradation under high-temperature conditions. Here, we propose a thermally and electrochemically stable high-valent iridium single atom synthesis strategy based on strong metal-support interactions (SMSI) to enhance high-temperature CO 2 electrolysis performance in solid oxide electrolysis cells (SOECs). The SMSI effect, in situ induced during high-temperature cell fabrication and operation, stabilizes the high-valent iridium single atom and simultaneously modulates the surface electronic structure of the La 0.6 Sr 0.4 FeO 3−δ (LSF) cathode by weakening the Fe−O hybridization, finally promoting oxygen vacancy formation and enhancing CO 2 adsorption and activation. This approach boosts the CO 2 -to-CO electrolysis current density by 80.8% relative to the pristine LSF cathode, achieving 3.02 A cm −2 at 800°C and 1.5 V with nearly 100% Faradaic efficiency and excellent stability over 600 h. These findings provide a viable strategy for designing thermally and electrochemically robust SACs for high-temperature catalytic reactions.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2026
·
IF 18.1
Huang Zhongnian,Wang Jundi,Ge Xiaohu,Lang Junyu,Cao Yueqiang,Wan Ying,Qian Gang,Yang Yong,Zhou Xinggui,Chen De,Yuan Weikang,Duan Xuezhi
CO 2 hydrogenation over earth-abundant Ni catalysts is attractive for CO-based fuel synthesis, but Ni intrinsically favors methanation. Here we show that ordered Ni 3 Sn 2 intermetallics tune Ni–CO electron back-donation and switch CO 2 hydrogenation from CH 4 formation to the reverse water–gas shift reaction. Atomic-resolution microscopy and X-ray absorption spectroscopy reveal disruption of extended Ni–Ni ensembles by Sn, while spectroscopy and theoretical calculations show that Ni–Sn d - p hybridization downshifts the Ni 3 d band and weakens Ni→CO 2π* back-donation. The Ni 3 Sn 2 catalyst achieves CO 2 conversion approaching thermodynamic equilibrium with nearly 100% CO selectivity and remains stable for 300 h. In situ infrared spectroscopy, steady-state isotopic transient kinetic analysis and theoretical calculations indicate that H-assisted CO 2 activation, spectator-like formate species and facile CO desorption underpin the CO-selective pathway. Similar behavior over Ni–Ga and Ni–In catalysts suggests a general back-donation strategy for redirecting Ni-based CO 2 hydrogenation.
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2025
·
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.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Xianglong Li,Haoxian Huang,Yachuan Yuan,Mingdong Wang,Xuanyu Cao,Yanbin Feng,Song Xue
Excessive CO 2 emissions have led to increasingly severe climate and environmental challenges. Within the framework of carbon neutrality, biological carbon fixation is a promising approach to improve the ecological environment and optimize energy systems. Salicylic acid decarboxylase (SAD) catalyzes the conversion of CO 2 and phenolic compounds into salicylic acid derivatives. However, the efficiency of CO 2 fixation in this process is low and is limited by the difficulty of product release during carboxylation. In this study, the engineered SAD, with the tunnel microenvironment remodeled to increase the turnover number ( k cat ), exhibited heightened CO 2 fixation efficiency. The mutant K23A/Y64T introduces a new tunnel architecture that indirectly enlarges the bottleneck radius of the native tunnel. These changes in the tunnel microenvironment facilitated product release, which was supported by evidence from both the catalytic activity and random acceleration molecular dynamics (RAMD). Kinetic analysis revealed that K23A/Y64T exhibited a 26-fold increase in catalytic efficiency ( k cat / K m ) with a K m consistent with that of the wild type, and the CO 2 conversion efficiency increased 14-fold. Dynamic cross-correlation matrices (DCCM) illustrated that α1 with K23A and loop5 with Y64T performed anticorrelated movements, enabling a change in the tunnel microenvironment between the two regions. Unlike conventional approaches targeting substrate–enzyme interactions, this study demonstrates that protein tunnel remodeling can intrinsically enhance carboxylation activity and holds potential for broad substrate applicability.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
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 .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
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.
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2025
·
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.
✓ 已验证
产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
·
2026
·
IF 7
Linlin Li,Jiang Zhao,Qingmei Ge,Yin-Hui Huang,Hang Cong,Wenfeng Zhao
Converting CO 2 into value-added chemicals using sustainable, biomass-derived catalytic systems is a key strategy for carbon mitigation and resource utilization. In this study, a heterogeneous biomass-derived zwitterionic polymer was fabricated from chitosan for CO 2 cycloaddition and N-methylation reactions. The synthesized porous bio-based polymer exhibits a robust structure and exceptional CO 2 adsorption capacity, leading to high catalytic efficiency. Under mild conditions, this catalyst achieved yields of up to 95% for 8 cyclic carbonates and 99% for 10 N-methylamines. Furthermore, the chitosan-based polymer demonstrates remarkable stability, maintaining its activity over at least 6 reuse cycles without significant degradation. Mechanistic studies indicate that the inherent –NH 2 or –OH groups on chitosan facilitate CO 2 and epoxide activation, while the zwitterionic structure provides active sites for ring-opening and cyclization processes.
✓ 已验证
产品关联
DOI
高影响因子
Carbon Capture Science & Technology
·
2026
·
IF 10.2
Shuo Xiang,Jun-Long Li,Tie Wu,Lian-Peng Li,Mian Hu,Jun Zhao,Zhong-Ting Hu,Zhiyan Pan
The growing demand for efficient carbon capture technologies has led to the exploration of biochar as a promising material for CO 2 adsorption, particularly through modifications such as nitrogen doping to enhance its performance. In this study, a series of biochars were prepared using different types of amine reagents and varying amounts of nitrogen doping. The highest adsorption capacity, 4.99 mmol g -1 , was achieved at 25 °C and 1.6 MPa when ethylenediamine was employed as the nitrogen source, with a mass ratio of the amine reagent to biochar of 1.2. Correlation analysis indicated that both physical and chemical adsorption significantly influenced CO 2 adsorption capacity. Additionally, by constructing biochar models with varying nitrogen contents and different nitrogen doping forms, theoretical calculations revealed that nitrogen doping could enhance the adsorption energy between CO 2 and biochar. This improvement in adsorption performance was more pronounced with higher nitrogen content. In this work, not only N-doped biochar with excellent CO 2 adsorption performance was prepared from waste biomass, but also the promotion mechanism of N-doped was revealed in detail by combining theoretical calculations and experiments.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）