APPLIED SURFACE SCIENCE
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2026
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IF 6.6
Shuangqian Liu,Liangshi Wang,Long Wang,Kun Zhang,Liang Xie,Yuxiang Li,Haiyang Zhang,Zongyuan Wang,Guixian Ge
The electrochemical CO 2 reduction reaction (CO 2 RR) to CO faces challenges from slow kinetics and complex pathways, necessitating active, selective, and stable catalysts. This study presents a direct coordination strategy that enables the in situ growth of cobalt tetranitrophthalocyanine (CoTNPc) on Co-embedded N-rich carbon matrix (Co/NC), forming a CoTNPc/NC composite. The directly axial coordination regulates the electronic configuration of Co-N sites, accelerating the *CO formation and desorption. The CoTNPc/NC electrocatalyst achieves a peak CO Faradaic efficiency for (FE CO ) of 96.7% at −0.9 V vs. RHE in H-cell. Furthermore, in the Flow-cell, it maintains FE CO > 90% over a wide potential range (−0.4 V to −0.9 V vs. RHE) and demonstrates durability exceeding 15 h in stability testing. In situ attenuated total reflection infrared (ATR-IR) spectroscopy and Density functional theory (DFT) calculations elucidate that the remarkable performance is driven by the improved electrical conductivity and weakened interaction between the *COOH intermediate and Co sites. This work offers a novel approach to optimizing catalyst-support interactions for electrocatalyst design.
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JOURNAL OF SUPERCRITICAL FLUIDS
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2026
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IF 4
Haixin Sun,Jianlei Qi,Jianzhong Yin
Currently reported Fe-NC catalysts for peroxymonosulfate (PMS) activation are mostly pyrolytically derived nanoparticle systems, which often suffer from low atomic utilization efficiency of the metal species. In this study, a single-atom Fe-NC catalyst was fabricated using a supercritical CO₂ deposition method, with iron(III) acetylacetonate as the metal precursor and a nitrogen-doped carbon material as the support. The as-prepared catalyst was employed to activate PMS for the degradation of Rhodamine B (RhB). Characterization by STEM, XRD, and BET analyses confirmed that the nitrogen-doped carbon support exhibits a high specific surface area and substantial nitrogen content. Aberration-corrected electron microscopy directly evidenced the uniform dispersion of isolated Fe atoms on the support surface. After 5 min of reaction, an RhB removal efficiency of 82.3% was achieved, corresponding to a turnover frequency of 2.73 min⁻¹. These results highlight the effectiveness of atomically dispersed Fe sites in activating PMS to generate reactive oxygen species.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2026
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IF 3.9
Zhangxinyu Fan,Yiheng Cui,Weixiang Wang,Yi Sun,Liqian Lin,Xinxin Geng,Guo Tian,Qin Zhong,Boyang Liu
Abstract Global warming has spurred interest in CO2 utilization. Coupling reverse water–gas shift (RWGS) with hydroformylation allows olefins to react with H2/CO2 to produce valuable aldehydes, which is a profitable reaction and helps with carbon fixation. However, temperature mismatch between the two reactions and limited mechanistic understanding hinder the rational design of catalysts. Using density functional theory (DFT) calculations and experimental evaluations, we investigated the effects of different phosphine ligands and acid additives on the performance of silane-free CO2 hydroformylation. Formic acid alters the CO2 activation pathway and reduces the energy barrier, thereby improving catalytic activity and chemoselectivity. The effects of reaction conditions reveal a competitive relationship between CO2 reduction and olefin carbonylation, suggesting that balancing RWGS and hydroformylation rates enhances catalytic performance. Our work not only deepens the mechanism understanding of silane-free CO2 hydroformylation but also paves the way for the rational design of subsequent high-performance catalysts.
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CONSTRUCTION AND BUILDING MATERIALS
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2026
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IF 8.9
Guolan Dou,Shuai Huo,Menghan Wang,Peng Chen,Xiaoxing Zhong,Botao Qin
A CO 2 uptake of 65.7 mg/g was achieved in the lignin-modified cementitious sealing material under a 30% CO₂ atmosphere. • A competitive microstructural mechanism of C-A-S-H decalcification and carbonate precipitation was proposed. • The carbonated lignin-modified cementitious sealing material retains both low permeability and high compressive strength. To integrate in-situ CO 2 sequestration with coal mine sealing and fire prevention, this study investigated the carbonation behavior and comprehensive sealing performance of a lignin-modified coal-based solid waste cementitious material (LFGS). Synthesized via the alkali activation of fly ash, coal gangue, and ground granulated blast furnace slag, the LFGS specimen was evaluated under varying CO 2 concentrations and carbonation durations, utilizing ordinary Portland cement (P·O 42.5) as a reference. Results indicate that the carbonation depth of the LFGS specimen follows a square-root-of-time relationship indicative of diffusion-controlled kinetics, demonstrating superior long-term CO 2 accessibility compared to P·O 42.5. After 28 days of exposure to 30% CO 2 , the CO 2 uptake of the LFGS specimen reached 65.7 mg/g. Furthermore, quantitative analysis confirmed that the low lignin dosage (0.1 wt%) exerts a negligible effect on the reactive calcium reservoir. Microstructural characterization revealed a competitive mechanism of matrix deconstruction and pore filling during carbonation. While the decalcification of C-A-S-H gel induces degradation and pore coarsening within its network, the concurrent precipitation of calcite and vaterite effectively fills capillary pores and microcracks. Despite this microstructural reorganization, the LFGS specimen retained a compressive strength of 29.8 MPa even after achieving a CO 2 uptake of 65.7 mg/g. This mechanical performance substantially exceeds that of conventional mine sealing materials. Crucially, the carbonated material maintained a low permeability coefficient, ensuring effective gas barrier properties. These findings demonstrate that the LFGS system fulfills the mechanical and permeability requirements for underground sealing operations while acting as a CO 2 sink, providing a viable pathway for the synergistic management of solid waste utilization, mine safety, and greenhouse gas mitigation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Yuchen Zhang,Xiaowei Zhou,ManMan Huo,Junfen Li,Yanfang Fan,Rong Zhang,Nanwen Li
Evaporation-rate control regulates kinetic trapping during polyimide membrane formation. • Stronger kinetic trapping preserves loosely packed nonequilibrium chain configurations with increased free volume. • Decarboxylative cross-linking amplifies structural gains, enhancing CO 2 permeability with modest selectivity loss. • This simple processing strategy improves CO 2 /CH 4 separation without polymer-backbone redesign or additional reagents. Kinetic trapping, the arrest of polymer chains in non-equilibrium configurations during rapid solvent evaporation, provides a deliberate route to engineer free-volume architecture in gas separation membranes. By controlling the solvent evaporation rate through casting temperature, faster evaporation from two solvents of contrasting volatility (DMAc and THF) systematically traps 6FDA-TFDB-DABA polyimide chains in more loosely packed configurations. This produces enlarged free volume, evidenced by expanded interchain spacing (5.33 to 5.49 Å, DMAc; 5.40 to 5.58 Å, THF), decreased density, enhanced birefringence, and increased surface roughness. This looser chain packing contributes to a substantial increase in CO₂ permeability, from 25.7 to 41.1 Barrer for DMAc-cast membranes and from 33.8 to 49.0 Barrer for THF-cast membranes, corresponding to increases of approximately 60% and 45%, respectively. These permeability gains arise from concurrent improvements in both CO₂ diffusivity and solubility, while the CO₂/CH₄ selectivity decreases only modestly. After thermal decarboxylation cross-linking at 340 °C, the rapidly evaporated THF-based membrane reaches 89.9 Barrer and surpasses the 1991 Robeson upper bound, withstanding feed pressures up to 600 psi without plasticization. This kinetic-trapping strategy requires no new reagents, monomer synthesis, or complex processing, offering a scalable, industrially compatible route to high-performance polyimide gas-separation membranes. Download: Download high-res image (280KB) Download: Download full-size image
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Industrial Chemistry & Materials
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2025
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IF 11.9
Hao-Ling Lan,Su-Tao Zheng,Li Xu,Guowei Guan,Qing-Yuan Yang
The separation of C2H2/CO2 mixtures for acetylene purification presents both industrial significance and fundamental challenges due to their nearly identical kinetic diameters and similar physical properties. This study demonstrates the effectiveness of ultramicroporous metal-organic frameworks (MOFs) in addressing this challenge through precise pore confinement effects. We report two ultramicroporous porous materials: Cu(cyhdc) (cyhdc2- = trans-1,4-cyclohexanedicarboxylate) and Cu(bdc) (bdc2- = 1,4-benzenedicarboxylate) and investigated their performance of capturing C2H2. At ambient conditions, both materials exhibit high C2H2 sorption capacities (1.92mmol g-1 for Cu(cyhdc) and 1.44mmol g-1 for Cu(bdc)). The most promising candidate is Cu(cyhdc), which shows decent C2H2 uptake capacity and a pretty high C2H2/CO2 selectivity (8.45 at 298K and 1 bar). Grand canonical Monte Carlo simulations revealed that the enhanced performance originates from multiple van der Waals interactions between C2H2 molecules and the curved cyclohexane-derived pore walls of Cu(cyhdc). Importantly, dynamic breakthrough experiments and scalable synthesis processes validated the practical separation potential of Cu(cyhdc) for C2H2/CO2 mixtures. This work provides both mechanistic insights into gas-framework interactions and a potential solution for energy-efficient acetylene purification.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Yifei Wang,Yingdong Yang,Yuxing Liu,Xinkang Zhang,Fengming Mo,Tao Huang,Yongjiang Shan,Ting Wu,Fei Zhang,Xiangshu Chen,Hidetoshi Kita
Capturing and recovering CO2 from steel industry gases is essential for environmental preservation since it lowers greenhouse gas emissions and raises CO concentrations. Because of its high selectivity, energy efficiency, and continuous operation, membrane separation technology has a lot of potential for CO2 separation. In the present work, a hydroxyl free radical (•OH), generated by the addition of a small amount of sodium persulfate to the precursor solution, was introduced for the first time to induce the synthesis of the ZSM-58 crystals and membranes. Hydroxyl free radicals can promote the depolymerization and condensation of silica sources during the synthesis process, thereby accelerating nucleation and crystallization. Compared with the precursor solution without sodium persulfate, the synthesis time of the membrane can be reduced by 30%, the resulting zeolite membrane exhibits a CO2/CO separation factor of 16 and a high CO2 permeance of 1.5 × 10–7 mol m–2 s–1 Pa–1. In addition, CO2/N2 and CO2/CH4 separation performances were also tested to evaluate the membrane quality. The separation factor of the equimolar CO2/N2 and equimolar CO2/CH4 mixtures reached 28.6 and 248.3 at 298 K at 0.1 MPa, accompanying the corresponding CO2 permeance of 1.3 × 10–7 mol m–2 s–1 Pa–1 and 1.5 × 10–7 mol m–2 s–1 Pa–1, respectively. This research presents an innovative and effective method for fabricating zeolite membranes.
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JOURNAL OF CATALYSIS
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2025
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IF 6.5
Jing Wang,Chengcheng Zhang,Huating Liu,Xusheng Wang,Songtao Zhang,Jinhua Ye,Li Shi
Doping semiconductor quantum dots (QDs) with heteroatoms has emerged as a technologically important tool for tuning their electronic structure and improving their photocatalytic activities; however, the resulting systems still suffer from low efficiency towards photocatalytic CO 2 reduction. Herein, we report that co-doping CdS QDs with Se 2- and Ga 3+ can boost the photocatalytic CO 2 reduction. The achieved CO evolution rate over Ga/Se co-doped CdS QDs is almost 20 times higher than that of pristine CdS QDs, and is also higher than some other reported QDs based photocatalysts for CO 2 photoreduction. The mechanism study uncovers that the co-doping of Se and Ga in CdS QDs can suppress the recombination of photogenerated electron–hole pairs and decrease the formation barrier of the key *COOH intermediate for promoting the CO 2 to CO conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Zhihong Liu,Jiale Liu,Jin Wang,Ping Lu,Shishun Xu,Yi Lu,Xiaofei Li,Qiaowen Zhang,Guocan Jiang,Zhengquan Li
The urgent need for clean energy has driven extensive research into efficient photocatalytic systems for CO 2 reduction. Lead-free Cs 3 Bi 2 Br 9 perovskites are particularly promising in this context, yet the photocatalytic performance of single-component Cs 3 Bi 2 Br 9 is often hindered by its narrow absorption in visible-light range. Here, we present a visible-to-near-infrared (vis-to-NIR) responsive Cs 3 Bi 2 Br 9 /Bi 19 Br 3 S 27 Z -scheme heterojunction photocatalyst, achieved by creating a high-quality interface upon in-situ growth. This heterojunction design markedly boosts CO₂-to-methane conversion, achieving electron consumption rates that are 70 and 124 times higher than those of pristine Cs 3 Bi 2 Br 9 and Bi 19 Br 3 S 27 , respectively. Mechanistic studies indicate that the formation of a strong built-in electric field at the interface facilitates efficient charge separation and transfer, significantly boosting photocatalytic performance. Notably, the photocatalytic performance of Cs 3 Bi 2 Br 9 /Bi 19 Br 3 S 27 heterojunction surpasses that of most lead-free halide perovskite photocatalysts. Our findings offer a new paradigm for interface engineering in photocatalysis and advance the development of vis-to-NIR responsive perovskites for sustainable energy conversion.
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PubMed
高影响因子
FUEL
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2025
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IF 7.5
Jingwen Lu,Sheng Su,Zhiwei Ma,Tao Liu,Kai Xu,Jun Xu,Long Jiang,Yi Wang,Song Hu,Jun Xiang
Fly ash (FA) has demonstrated cost-effective potential for CO 2 capture, yet its practical application is hindered by inadequate pore structure and complex processing. Chitosan (CS), a polysaccharide rich in amine groups, offers distinct advantages as it enables straightforward synthesis of adsorbents without requiring high temperature/pressure or templates, and provides regular pores, making it an ideal candidate for modifying FA to enhance its pore structure and streamline the preparation process. Therefore, the adsorbent of polyethyleneimine(PEI)-impregnated FA modified by CS was developed to investigate CO 2 adsorption performance at different conditions. The properties and mechanisms were characterized by XRD, SEM, FT-IR etc. Characterization results revealed that the introduction of CS transformed the irregular macropores of FA adsorbents into ordered three-dimensional networks, significantly improving the pore structure and specific surface area, while introducing amine groups from CS into the adsorbents. The FA/CS 1 -50PEI achieved a maximum CO 2 adsorption capacity of 1.96 mmol/g (40 °C, 100 mL/min and 15 % CO 2 ) in experiments. After 10 adsorption–desorption cycles (40 °C, 200 mL/min and 15 % CO 2 ), it retained 93 % of initial adsorption performance, demonstrating exceptional stability and effectioncy for CO 2 adsorption. DRIFTS analysis confirmed the successful introduction of amine groups from CS, and the appearance of carbamate’s specific peak at different wavenumbers further validated the involvement of amine groups in CS and PEI in the adsorption process. Additionally, adsorption kinetic analysis revealed the adsorption mechanism involved both physisorption and chemisorption. It also confirmed that CS not only provided regular pores for PEI impregnation, but also the amine groups in CS exposed to the pore surface participate in adsorption reaction with the that in PEI.
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ACS Sensors
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2025
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IF 9.1
Zuorong Huang,Quanquan Tang,Jing He,Lei Wu,Fengmin Liu,Xishuang Liang,Bin Wu,Mingliang Fu,Geyu Lu
Diesel engines in the field of transportation are one of the important sources of carbon dioxide (CO2) emissions, and incomplete combustion and complex working conditions make it difficult to accurately calculate their CO2 emissions by using the intake volume. In addition, the high temperature and harsh environment of exhaust gas also put higher requirements on the response speed, stability, and high-temperature resistance of the sensor. In this study, Co3O4 was doped into the auxiliary phase Na2CO3 as a catalyst and stabilizer to improve the sensor sensitivity, and solid electrolyte NASICON was doped to improve the sensor response speed. The results show that when the doping ratio of Na2CO3 and NASICON is the same as 10 wt %, the response to CO2 of 5000 ppm can reach −67 mV, and the full-range second-level response to CO2 is realized. The detection range is up to 0–180,000 ppm, the sensitivity is −64 mV/decade, the sensor has good selectivity to CO2, the response change in the range of 20–98% RH is negligible, and the response change in 60 days is only −8.66%. This sensor had good reproducibility. In addition, the in situ on-board CO2 sensing probe and test system were developed. The sensor response was calibrated against the measurement values of standard instruments on the entire vehicle. Based on the calibration results, a regression curve was established and the vehicle was tested; the test results and the standard instrument test value deviation are basically less than 10% to verify the practicality of the component in the exhaust gas detection.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yaqi Liu,Jie Jiang,Yun Ju,Jing He,Hong Zhang,Jing Zhao,Lina Qiao
Pyruvate, serving as a bridge between the linear acetyl coenzyme A (acetyl-CoA) and the reductive tricarboxylic acid (rTCA) cycle, is of prime importance for life evolution. However, the carboxylation of pyruvate with carbon dioxide (CO 2 ) followed by coupling into the rTCA cycle remains challenging in prebiotic chemistry. Here, we present that pyruvate spontaneously undergoes carboxylation with CO 2, giving oxaloacetate, malate, and fumarate of the rTCA cycle in water microdroplets at room temperature without catalysts. The current pathway that pyruvate directly uses CO 2 as a carbon source depends on the microdroplet surface, distinct from the previously reported pathway using glyoxylate. These findings suggested that pyruvate may have participated in the cycle of enzyme-free carbon fixation on a prebiotic Earth. Furthermore, the widespread microdroplets in the atmosphere may also have acted as a potential synthesis setting for CO 2 fixation and utilization. This offers a promising strategy for climate change control and the promotion of sustainable carbon cycling in the future.
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