ACS Nano
·
2026
·
IF 17.3
Zezhong Xie,Jinli Yu,Hao Yang,Jian Chen,Muzi Yang,Mingyang Li,Kun Wang,Qiushi Wang,Kai-Hang Ye,Gangfeng Ouyang
The solid–liquid–gas triple-phase interface in the CO2 electro-reduction reaction (CO2RR) is pivotal for determining catalytic activity and selectivity, as it influences both the kinetics and thermodynamics of the reactions. However, observing this interface in situ is challenging because it forms at the interface among the solid catalyst, the flowing electrolyte, and the turbulent CO2. To address the issues, we achieved unobstructed in situ Raman observations at the microscale by developing a straightforward catalyst-integrated gas diffusion electrode (GDE). This monolithic GDE, featuring a biomimetic hydrophobic structure, fully releases the triple-phase interface─an essential prerequisite for enabling the in situ detection. Characterizations reveal that the microenvironment at the triple-phase interface significantly enhances multicarbon (C2+) selectivity. Furthermore, using advanced in situ 3D Raman tomography, we successfully visualized the spatial distribution of the triple-phase interface with high precision. The integration of in situ Raman spectroscopy with computational modeling has provided invaluable insights into the evolution of species within the microenvironment, elucidating a high local pH and rapid CO2 mass transfer at the triple-phase interface.
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PubMed
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.
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Sustainable Chemistry and Pharmacy
·
2026
·
IF 5.8
Gao Rui,Xu Bingqi,Gao Weichen,Jiang Ping,Zhang Shiyu,Cui Kai,Zhao Yingliang
Alkali-activated slag (AAS) binders activated solely by sodium hydroxide often exhibit poor performance, requiring additional sodium silicate, which increases both cost and environmental impact. To overcome these limitations, in this study, a novel CO 2 -assisted activation (CAA) strategy, integrating CO 2 mineralization with mechanical activation, is proposed to enhance the performance of AAS binders. Reaction kinetic modeling revealed that the slightly lower reaction order observed in the CAA-treated AAS system, reflects a suppression of diffusion-controlled hydration, which in turn prolonged the nucleation-growth stage and enabled a uniform hydration pathway. Structural analysis suggests enhanced silicate polymerization in CAA-treated AAS samples, as evidenced by increased Q 2 (1Al) content, mean chain length, and polymerization degree from 29 Si NMR. These gel-level refinements resulted in a denser and more cohesive matrix, contributing to improved mechanical performance. Specifically, the optimized system exhibited a 68.0 % increase in 1-day compressive strength and a 45.6 % enhancement at 28 days, along with reduced porosity and higher micromechanical stiffness. The synergy between CO 2 and the mechanical activation in CAA process suggests that CO 2 acts as a field-enhancing agent, modifying the physicochemical environment and promoting nucleation processes. Overall, this work demonstrates that CAA offers a dual-function strategy—both chemical and environmental—for designing high-performance, low-carbon AAS systems.
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Carbon Energy
·
2026
·
IF 24.2
Fengyu Tian,Yaohao Li,Xuemin Yan,Huiwen Zhu,Jiayu Liang,Honglei Zhang,Ning Han
Photocatalytic CO 2 reduction involves multiple proton-coupled and multi-electron transfers, leading to a plethora of reaction pathways and consequently unpredictable products. The unique electronic structure and unsaturated coordination environment of single-atom photocatalysts can influence the reaction pathways of CO 2 photoreduction, enhancing the yield of a target product. Herein, we rationally design the In single-atom photocatalyst (In-NTO) containing isolated In δ+ –N 3 O 2 atomic interface sites for highly efficient and selective CO 2 -to-CO photoreduction. This distinctive atomic configuration not only reduces the overall activation energy barrier but also transforms the key *CO desorption step from an endoergic to an exoergic one, thereby altering the reaction pathway to selectively produce CO rather than CH 4 . Consequently, the 0.25 wt% In-NTO exhibits high selectivity (95.9%) for photocatalytic CO 2 -to-CO conversion, with a rate of 6.34 µmol g −1 h −1 . This work offers a novel strategy for modulating the reactivity and product selectivity of photocatalytic CO 2 reduction toward desired products by constructing single-atom sites with heteroatomic coordination.
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高影响因子
CATALYSIS LETTERS
·
2026
·Vol. 156
·期 2
·50
·
IF 2.4
Cheng Hongna,Wang Chaoyong,Wang Zihan,Peng Weikang,Hou Jiayi,Tian Shiting,Shi Zixuan,Liu Ying,Li Fengfeng,Zhang Mingxi
The climate crisis caused by excessive carbon dioxide (CO 2 ) emissions urgently call for efficient electrocatalytic reduction technology to convert CO 2 into high value-added products. In this study, nickel polyphthalocyanine (NiPPc) electrocatalysts with different copper (Cu) doping amounts (10–90 wt%) were prepared by solvothermal method, Combining X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and other characterization and electrochemical testing, it is found that: Doping with 10 wt% Cu significantly enhanced catalytic activity, achieving a current density of 325 mA cm −2 at − 0.6 V (vs. RHE)—2.8 times that of the sample; 50 wt% Cu doping optimized the Cu–N 4 active sites, yielding a carbon monoxide (CO) Faraday efficiency of up to 95% at − 1.0 V; 30 wt% Cu-doped catalyst can generate CO: H 2 = 1:1 syngas, A controllable catalyst design strategy is provided for CO 2 electrocatalytic reduction. Graphical Influence of Cu Loading (10–90 wt%) on Electrocatalytic CO 2 Reduction Activity and CO Selectivity of NiPPc Catalysts.
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
·
2013
·Vol. 51
·期 13
·2834-2840
·
IF 3.543
Lin Gu,Yusheng Qin,Yonggang Gao,Xianhong Wang,Fosong Wang
Common CO 2 -based biodegradable polycarbonates like poly(propylene carbonate) or poly(cyclohexene carbonate) are generally hydrophobic, leading to slow biodegradation rate and poor cell adhesion, which limit their applications in the biomedical field. Here hydrophilic polycarbonates were prepared by one-pot terpolymerization of CO 2 , propylene oxide (PO), and 2-((2-(2-(2-methoxyethoxy)ethoxy)ethoxy)methyl)oxirane (ME 3 MO) using binary Salen Co(III)-Cl/PPNCl catalyst system. The resultant terpolymers showed one glass transition temperature ( T g ), which decreased with the increase of ME 3 MO units in the terpolymers ( F ME3MO ). Water contact angles of the resultant terpolymers with F ME3MO of 4.2−23.6% were 68−25°, while that of poly(propylene carbonate) was 90°, indicating that the terpolymers became hydrophlilic. Furthermore, the terpolymers with F ME3MO more than 25.8% exhibited reversible and rapid thermo-responsive property in water, and the lower critical solution temperature (LCST) was highly sensitive to F ME3MO . In particular, aqueous solution of the terpolymer with F ME3MO of 72.6% showed a LCST around 35.2 °C, close to body temperature, which was promising for biomedical applications, especially for in vivo applications. © 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2013, 51, 2834–2840.
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高影响因子
FUEL
·
2022
·
IF 8.035
Yongtao Zhang,Fulin Chen,Yan He,Fei Wang
CO 2 sequestration based on hydrate technology is considered to be the most promising long-term CO 2 sequestration technology. In this study, a method of using initial stirring to activate CO 2 hydrate formation process was proposed in the aim of saving energy and avoiding the problem of stirring shaft stuck, where the stirring only played a role in activating hydrate formation process. Two amino acids, l -Methionine and d -leucine, were chosen as promoters for improving the formation kinetics of CO 2 hydrates, and l -Methionine presents better than d -leucine. When the concentration of l -methionine solution is equal to or greater than 4 mmol/L, even with the initial stirring of 10 rpm within 8 min, T 90 can be shortened to close to or less than 40 min with a high gas consumption of more than 7.3 mmol gas/mL water, where the promoting effect is similar to the condition of continuous stirring of about 100 min, indicating that about 90 % of the energy consumed for mechanical stirring can be saved. Moreover, an interesting phenomenon was observed that CO 2 hydrates firstly nucleated inside the l -methionine solution, and a large number of small hydrate floccules rapidly formed and filled the entire solution under the action of magnetic stirring, which proved the instantaneous excitation effect of stirring on hydrate formation. This work contributes to rethinking the promoting roles of stirring and promoters in CO 2 hydrate formation.
研究领域:
环境科学
·
能源化学
·
物理化学
·
气体水合物
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碳捕集与封存
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2017
·Vol. 134
·期 28
·45046
·
IF 1.86
Fenglei Liu,Shuixia Chen,Yanting Gao,Yufang Xie
A solid amine adsorbent was prepared by modifying a porous polystyrene resin (XAD-4) with chloroacetyl chloride through a Friedel–Crafts acylation reaction, followed by aminating with tetraethylenepentamine (TEPA). The adsorption behavior of CO 2 from a simulated flue gas on the solid amine adsorbent was evaluated. Factors that could determine the CO 2 adsorption performance of the adsorbents such as amine species, adsorption temperature, and moisture were investigated. The experimental results showed that the solid amine adsorbent modified with TEPA (XAD-4-TEPA), which had a longer chain, showed an amine efficiency superior to the other two amine species with shorter chains. The CO 2 adsorption capacity decreased obviously as the temperature increased because the reaction between CO 2 and amine groups was an exothermic reaction, and its adsorption amount reached 1.7 mmol/g at 10 °C in dry conditions. The existence of water could significantly increase the CO 2 adsorption amount of the adsorbent by promoting the chemical adsorption of CO 2 on XAD-4-TEPA. The adsorbent kept almost the same adsorption amount after 10 cycles of adsorption–desorption. All of these results indicated that amine-functionalized XAD-4 resin was a promising CO 2 adsorbent. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 45046.
研究领域:
环境化学
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高分子材料科学
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气体吸附与分离
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碳捕集技术
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高影响因子
Journal of CO2 Utilization
·
2019
·
IF 5.189
Wei Zhang,Fengzhen Zhang,Liping Ma,Jing Yang,Yi Wei,Deqi Kong
In this work, we propose a novel, effective, energy efficient technology to reduce CO 2 emissions and fully use the calcium in the solid waste by-product phosphogypsum (PG), by capturing CO 2 from the PG decomposition product’s hydrolysis solution. Experiments were conducted to investigate the technical feasibility and the influence of temperature and CO 2 partial pressure on CO 2 capture, as well as CO 2 loading on CO 2 sorption capacity. The results showed that > 90 % of the total calcium ions in the solution were converted into calcium carbonate (CaCO 3 ). Furthermore, a decrease in temperature and an increase in CO 2 partial pressure improved CO 2 uptake, with the latter having a greater effect on CO 2 capture capacity than the former. Moreover, kinetic analysis demonstrated that a higher temperature and CO 2 partial pressure increased the absorption rate; and showed that the CO 2 absorption rate is highly affected by the CO 2 loading levels. The thermodynamic analysis indicated that CO 2 absorption heat significantly declined as a function of increasing CO 2 loading. CaO from the calcination of carbonate was added to the hydrolysis solution and significantly enhanced its CO 2 capture ability. Thus, the hydrolyate of PG decomposition products in combination with CaO reinforcement may be a promising method for CO 2 capture.
研究领域:
环境化学
·
工业生态学
·
固废资源化
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碳捕集与封存
·
过程强化
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2019
·Vol. 136
·期 27
·47723
·
IF 2.188
Yayun Zheng,Yaofang Hu,Xing Yang,Meng Yuan,Jie Zhang,Yaodong Zhang,Jujie Luo
We synthesized novel polyurethane (PU) membranes from isophorone diisocyanate (IPDI), poly(ethylene glycol) (PEG) with a molecular weight of 2000, aminopropyl-terminated poly(dimethyl siloxane) (PDMS) with a molecular weight of 2000, and 1,4-butanediol (BDO) via a two-step polymerization. The structure of each synthesized membrane was studied through Fourier transform infrared spectroscopy and gel permeation chromatography. The effect of the thermal behavior was determined by differential scanning calorimetry and thermogravimetric analysis. The gas-permeability characteristics of the PU membranes were then tested for a single gas. The results show that the permeability of CO 2 ( P CO2 ) gradually increased with PDMS content. Among these PU membranes, PU-d (PEG/PDMS = 1:1, PEG/PDMS/IPDI/BDO = 1:3:2) showed the best P CO2 (132.6 Barrer) at 25°C and 1 bar pressure. The gas-permeability coefficients of each PU membrane at different operating temperatures were investigated, and the results show that P CO2 reached 302.6 Barrer at 65°C and 1 bar. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47723.
研究领域:
高分子材料科学
·
膜分离技术
·
气体分离
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功能高分子
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环境化工
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Ningyuan Zhang,Chengxu Li,Xiao Cui,Ye Ma,Yanhang Ma,Ning Wang,Qiming Sun
A universal physical-mixing strategy boosts formic acid dehydrogenation over supported Pd catalysts. • Basic zeolites scavenge CO 2 to enhance formic acid dehydrogenation. • Pd@S-1/1.0CsX achieves a hydrogen production rate of 4269 h −1 . • A CO 2 -deficient microenvironment exposes Pd sites and drives hydrogen evolution. Formic acid dehydrogenation (FAD) is an attractive route for hydrogen release in liquid organic hydrogen carrier systems, but its efficiency is often limited by product accumulation at metal active sites. Herein, we report a simple yet highly effective mixing strategy that markedly enhances FAD by integrating zeolite-encaged Pd nanoclusters with basic zeolites. The resulting bifunctional catalytic system combines the intrinsic activity of subnanometric Pd nanoclusters with the CO 2 -scavenging capability of basic zeolites. As a representative example, the Pd@S-1/1.0CsX catalyst achieves a hydrogen production rate of 4269 h −1 , nearly threefold higher than that of Pd@S-1. Mechanistic investigations indicate that the basic zeolite acts as a local CO 2 sink, dynamically promoting the transfer of newly generated CO 2 away from the Pd/liquid interface and thereby maintaining a CO 2 -deficient microenvironment around the active Pd sites. This interfacial CO 2 scavenging suppresses product readsorption and local product inhibition, continuously exposing accessible Pd sites without altering the intrinsic reaction pathway. The generality of this strategy is demonstrated across a broad range of supported Pd catalysts. This work highlights microenvironment engineering as a powerful concept for advancing heterogeneous catalysis beyond conventional active-site-centered design. Zeolite-encaged Pd nanoclusters are physically mixed with basic zeolites to create a bifunctional catalyst for formic acid dehydrogenation. The basic zeolite scavenges CO 2 , generating a CO 2 -deficient microenvironment that continuously exposes Pd active sites, shifting equilibrium toward H 2 evolution and delivering nearly threefold higher H 2 productivity. Download: Download high-res image (106KB) Download: Download full-size image
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Xi Tang,Bin Xu,Xiaoyi Gao,Xiaoshan Li,Ge Gao,Wen Chen,Fan Wu,Cong Luo,Liqi Zhang
A multi-criteria rapid preliminary screening method for absorbents has been proposed. • Quasi-cycle capacity, absorption heat, and boiling point indicators were highly important for amine absorbents. • TEDA-DMEN exhibited a large quasi-cycle capacity, a low CO 2 absorption heat, and a low cost. The core of the CO 2 capture technology based on chemical absorption lies in the optimization of the performance of the absorbent. However, the current methods and indicators used to evaluate the performance of absorbents are limited, particularly those that incorporate energy consumption. This paper proposes a multi-criteria rapid preliminary screening method for absorbents, covering seven key indicators of the amine absorbent for CO 2 capture, to characterize CO 2 reaction performance, energy consumption performance, physical properties, and economic performance. The Analytic Hierarchy Process (AHP)-entropy weight Technique for Order Preference by Similarity to Ideal Solution (TOPSIS) method was used to rapidly screen 18 amine absorbents in three categories. The results showed that the evaluation method was primarily suitable for aqueous amines and could also be extended to other types of absorbents. In addition, the combined subjective and objective weighting results indicated that the quasi-cycle capacity, absorption heat, and boiling point indicators were highly important for amine absorbents. The comprehensive index (CI) demonstrated that among the three amine categories, AEEA, PS, and TEDA-DMEN were the best absorbents for CO 2 capture, respectively. In particular, TEDA-DMEN exhibited a large quasi-cycle capacity (0.560 mol/mol), as well as low CO 2 absorption heat (66.87 kJ/mol), sensible heat (37.61 kJ/mol), and cost (0.104 $/g). This paper provides a theoretical basis and methodological support for developing high-efficiency, low-energy, and low-cost absorbents for CO 2 capture.
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