CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Li-Ning Dong,Cunmin Wang,Le Bao,Kun Yu,Yuzhen Hou,Xinjian He,Mengbao Fan,Shenghui Zhang,Shu-Gui Yang,Jiefeng Gao,Huan Xu
Biodegradable poly(lactic acid) (PLA) nanofibrous membranes (NFMs) alleviate plastic pollution and attract attention in particulate matter (PM) filtration. However, they lack gas selectivity, and their poor electroactivity coupled with rapid charge dissipation leads to unstable PM filtration efficiency, which hampers their further development. Herein, we employed a microwave-assisted method to fabricate high-selectivity active nanocrystals (HSANs), and integrated them into PLA NFMs via a combined electrospinning-electrospray strategy, yielding HSA-PLA NFMs with a hierarchical porous structure. With uniform HSANs anchoring (3, 6 and 9 wt%), the obtained HSA-PLA NFMs showed increased surface potential (up to 8.3 kV), dielectric constant (1.71) and porosity (95.6 %). They exhibited excellent CO 2 adsorption and HSA-PLA9 reached 1.9 mmol·g −1 at 273.15 K/1.0 bar. Its CO 2 /N 2 selectivity was confirmed by IAST/breakthrough tests and the mechanism analyzed via three isothermal models. Moreover, endowed with pronounced activity and optimized morphology, HSA-PLA NFMs exhibited PM 2.5 and PM 0.3 filtration efficiencies of 99.7 % and 99.3 % at 85 L/min, remarkably outperforming Pure PLA (only 84.9 % and 83.9 %). This strategy integrates CO 2 adsorption and PM filtration, thereby facilitating the development of eco-friendly multifunctional permselective membranes for simultaneous purification.
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Journal of Materials Chemistry A
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2025
·
IF 9.5
Lili Wan,Linxiao Wu,Yumeng Han,Fusong Kang,Dongfeng Du,Jinshui Cheng,Jingshan Luo
Efficient and selective photoelectrochemical CO2 reduction remains a significant challenge for solar fuel production. Here, we fabricated a heterostructured Cu2O photocathode featuring a pristine SnO2 layer deposited via atomic layer deposition. Upon photoelectrochemical activation, the SnO2 layer transformed into uniformly distributed Sn/SnOₓ nanoparticles across the photocathode surface. Systematic characterization revealed the SnO2 layer's structural evolution. The activated Cu2O photocathode significantly enhanced the charge transfer characteristics and PEC CO2 reduction performance, delivering a current density of -2.5 mA cm-2 at -0.2 V vs. RHE and a formate Faradaic efficiency of 75.4% at -0.1 V vs. RHE. Coupling with a semitransparent BiVO4/NiCo LDH photoanode enables unassisted, solar-driven CO2 reduction and ethylene glycol (EG) oxidation, achieving a current density of 0.11 mA cm-2 and producing 0.13 μmol cm-2 formate yield in the first 0.5 hour. This work presents a scalable and earth-abundant materials-based strategy for efficient PEC CO2 reduction and underscores the potential of tandem architectures for sustainable solar fuel generation.
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JOURNAL OF CATALYSIS
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2025
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IF 6.5
Shengyao Zhou,Ming Zheng,Meiyue Cheng
The electrocatalytic CO 2 reduction reaction (CO 2 RR) using renewable electricity emerges as a promising route for carbon neutralization, which has attracted numerous attentions in recent years. Regulating the micro-environment surrounding the reaction interface is of great importance for selective CO 2 electroreduction but remains challenging. This study employed the potassium chloride (KCl) electrolyte to regulate the micro-environment surrounding the silver nanowires (AgNWs) catalyst for efficient electrocatalytic CO 2 -to-CO conversion. Rather than focusing on the effect of individual anions or cations in CO 2 RR, as previously reviewed elsewhere, we herein elucidated the effect of both Cl − and K + on the micro-environment surrounding the active centers. Experimental results and DFT calculations revealed that K + could facilitate the CO 2 adsorption and activation, while Cl − could promote *COOH formation and suppress HER. Findings from this study may provide new insights into the micro-environment engineering for efficient CO 2 RR.
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ACS Catalysis
·
2025
·
IF 13.1
Kaidi Zhang,Hai Wang,Rui Tang,Yuan Huang,Yating Lv,Huixin Wu,Qingsong Luo,Wentao Yuan,Yong Wang,Liang Wang,Feng-Shou Xiao
Catalytic hydrogenation of carbon dioxide (CO2) into carbon monoxide (CO) is a key process during the CO2 conversion into high-value chemicals but lacks stable and selective catalysts due to catalyst deactivation from surface restructuring under the reaction conditions. We showed that the supported Rh catalyst modified with titanium oxide overlayers (Rh@TiOx/TiO2) offered nearly full selectivity for conversion of CO2 to CO in a wide reaction temperature window, gas space velocities, and H2/CO2 ratios. The high CO selectivity was maintained even after treating the Rh@TiOx/TiO2 catalyst in oxidative, reductive, and humid atmospheres, giving good stability for 500 h at 500 °C. Kinetic studies and characterizations of the catalysts reveal that the high selectivity and stability result from the hindered CO-Rh interactions and stable Rh-TiOx interfaces. Similarly, supported Pd and Pt catalysts (Pd@TiOx/TiO2 and Pt@TiOx/TiO2) were also successfully prepared, which showed high CO selectivity and good stability in selective CO2 hydrogenation, providing a generalized route for the preparation of highly stable and selective hydrogenation catalysts.
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CHEMICAL PHYSICS
·
2025
·
IF 2.4
Qiqi Niu,Yiqi Pan,Ming Chen,Longfei Sun,Kang Zhang,Yun Zhang,Jing Yan,Wei Qi,Lin Yang,Zhaoxia Dong,Xiaochen Li
CO 2 foam plays a pivotal role in the synergistic integration of enhanced oil recovery and carbon geological storage, which is attributed to its ability to control CO 2 mobility and accelerate CO 2 dissolution-mineralization. However, foams are inherently thermodynamically unstable systems. Notably, CO 2 not only undergoes inter-bubble diffusion but also dissolves in aqueous phases, collectively exacerbating foam destabilization. Therefore, it is of great significance to optimize the structure of the foam agent for constructing a highly stable CO 2 foam system. In this paper, the properties of CO 2 bubble film and the arrangement of molecules on the liquid film were studied through experiments and molecular simulations in a series of conventional surfactant solutions. Specifically, the effects of hydrophobic carbon chains and hydrophilic groups of surfactants on liquid film permeability, interfacial adsorption process, bubble stability, and CO 2 molecular behavior were analyzed. The lab results show that the CO 2 bubbles in systems containing C16-based quaternary ammonium (TAC-16) and betaine (S16) surfactants exhibited lifespans of 186 and 69 min, respectively, representing 85 and 29 times longer than that of C12-based counterparts (TAC-12 and S12). The liquid film permeability of CO 2 bubbles in TAC-16 and S16 were 5.02 and 11.99 cm/min, corresponding to 1/7 and 1/3 of TAC-12 and S12. Furthermore, the adsorption capacities of TAC-16 and S16 were 1.63 and 3.06 mol/m 2 at the gas-liquid interface, which were greater than those of TAC-12 and S12. Long-chain surfactants had strong hydrophobic interactions, which enhanced their adsorption and micelle formation capabilities. Long-chain surfactants showed a certain affinity for CO 2 molecules and could form a dense adsorption layer at the gas-liquid interface. The results indicate that the long-chain surfactants can delay the diffusion and dissolution of CO 2 in the liquid film and have obvious advantages as CO 2 foam agents. This work preliminarily reveals the molecular states and interactions within CO₂ foams, providing critical insights for designing and developing CO 2 foam agents.
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Minerals
·
2025
·Vol. 15
·期 5
·506
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IF 2.2
Xiaoyu Li,Jie Chen,Wenqing Zhang,Chenyu Wang,Hui Ma,Kang Peng,Zheng Zhou
The urgent need for efficient CO2capture technologies has driven research into amine-functionalized adsorbents, though existing methods face trade-offs between adsorption capacity and cycling stability. This study addresses these limitations by developing a novel hybrid modification strategy combining chemical grafting and physical impregnation on polymorphic kaolinite minerals. Through systematic acid leaching and hybrid grafting–impregnation amine functionalization, the adsorbents with hierarchically porous structures and optimized performances are synthesized. The tubular adsorbent (ATK-APTES-PEI) demonstrated exceptional performance, achieving a CO2uptake of 1.68 mmol/g at 75 °C under a 60% CO2/40% N2mixed gas flow, with only 5.3% capacity loss after 10 adsorption–desorption cycles, significantly outperforming both rod-like (ARK-APTES-PEI, 1.55 mmol/g) and flake-like (AFK-APTES-PEI, 1.23 mmol/g) variants. The unique pore structure of ATK-APTES-PEI enables simultaneous high amine loading and maintained gas diffusion pathways, while the hybrid modification strategy synergistically enhances both adsorption capacity and stability by increasing active surface sites. These findings establish critical structure–property relationships for mineral-based adsorbents and demonstrate a scalable approach for industrial CO2capture applications. The work provides a blueprint for designing cost-effective, stable adsorbents using abundant clay minerals, bridging materials science with environmental engineering for sustainable carbon management solutions.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yanni Ran,Kang Peng,Ziyan Li,Xingwang Guo,Honglin Chen,Shengxuan Cai,Lei Su,Min Niu,De Lu,Hongjie Wang
CO 2 capture can mitigate carbon emissions with the objective of achieving carbon neutrality. Solid amine adsorbents have emerged as one of the most promising materials for capturing CO 2 . However, balancing the diffusion and adsorption of CO 2 remains a significant challenge, making it difficult to achieve high capacity and rapid kinetics simultaneously. In this study, SiC nanowires aerogel (SiCNWA) was functionalized with tetraethylenepentamine (TEPA) and diethanolamine (DEA) for CO 2 capture. The optimal adsorbent was synthesized with a total amine loading of 90 wt%, comprising 75 wt% TEPA and 25 wt% DEA. It exhibits a high CO 2 adsorption capacity of 4.71 mmol/g and ultra-rapid adsorption kinetics, achieving 80 % adsorption capacity within the first minute. The advantageous properties stem from the synergistic effects arising from the unique three-dimensional network structure of SiCNWA, coupled with the complementary group interactions of the hybrid amines. The ultra-high porosity of aerogel facilitates a high proportion of amine loading and dispersion, contributing to its high CO 2 adsorption capacity. Additionally, the continuous network structure offers efficient channels for CO 2 transport, enabling ultra-rapid CO 2 adsorption kinetics. The high amine density of TEPA provides abundant adsorption sites for CO 2 , and the addition of DEA can effectively mitigate the aggregation and deactivation of amine groups, thereby significantly improving the adsorption rate and adsorption capacity. This aerogel-hybrid amines strategy effectively balances diffusion and adsorption, offering valuable insights for advancing aerogel-based materials for CO 2 capture.
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ACS Catalysis
·
2025
·
IF 13.1
Da Wang,Guangbo Liu,Chuanhui Zhang,Chao Feng,Jinhu Wu,Song Chen,Wenjie Xiang,Hao Huang,Zhihao Liu,Noritatsu Tsubaki
The reasons for the too high CO2 selectivity (near 50 C %) in Co2C-based Fischer–Tropsch to olefins (FTO) are not clear. Water–gas-shift (WGS) side reaction is thought to be responsible for this, but in-depth research is lacking. Here, we revealed the mechanism of the too high CO2 selectivity in Co2C-based FTO. Kinetic studies showed that WGS reaction was more likely to occur than the hydrocarbon production reaction. In addition, a too severe WGS reaction would result in the formation of an H2-enriched and CO-deficient environment on the catalyst surface, which was not favorable for the generation of light olefins. Catalyst characterization results proved that the severe WGS reaction could also lead to the transformation of prismatic Co2C to spherical Co2C. Theoretical calculations demonstrated that prismatic Co2C (020) and Co2C (101) facets were dominant crystal facets for both FTO and WGS reactions. Furthermore, in situ diffuse reflectance infrared Fourier transform spectroscopy experiments found that the H2O produced in FTO completely participated in the WGS reaction. This clearly revealed why the CO2 selectivity was close to 50 C % in FTO. Therefore, we believed that accelerating the desorption of H2O on the catalyst surface and preventing its readsorption are the key elements for inhibiting CO2 formation in FTO.
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RSC Advances
·
2025
·Vol. 15
·期 17
·13313-13322
·
IF 4.6
Hengxin Ren,Xinyu Sun,Tong Li,Zhixin Ren,Chaoyu Song,Yuguang Lv,Ying Wang
Herein, a new Z-scheme BiVO4/Cu2O/PPy heterostructure photocatalyst was developed with bismuth nitrate and ammonium vanadate as the precursors and sodium dodecyl benzyl sulfonate as the soft template. Through the spatial confinement effect of the sodium dodecyl benzyl sulfonate soft template, peanut-like BiVO4 and the BiVO4/Cu2O/PPy heterojunction were synthesized. The best performance was observed for BiVO4/Cu2O/PPy (5%), and its photodegradation rate was 6.57 times higher than that of pure BiVO4. The mechanism study showed that a light hole (h+), superoxide radical (·O2−), and hydroxyl radical (·OH) participated in the CO2 reduction process, which was different from the pure BiVO4 reaction system. Therefore, the proposed approach provides a new method for applying BiVO4/Cu2O/PPy photocatalysts and developing the same type of heterojunction photocatalyst, and they have effective practical application for environmental remediation.
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PubMed
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ACS Catalysis
·
2025
·
IF 13.1
Shaorong Deng,Chenji Zhu,Xiuzhong Fang,Xianglan Xu,Xiang Wang
A series of Ru-x%Li+/SiO2 catalysts (x = 0.05–0.2), modified with varying amounts of lithium cation (Li+), were prepared via coimpregnation and evaluated for CO2 methanation to explore Li+ modification on Ru/SiO2. Introducing trace Li+ markedly boosts reaction activity, with the optimal Ru-0.1%Li+/SiO2 exhibiting 38.4 and 12.3 times higher overall reaction rate and turnover frequency at 200 °C, respectively, compared to Ru/SiO2. Structural characterization confirmed that Li+ incorporation effectively suppresses RuO2 crystallization, thereby improving Ru dispersion from 9.1% to 31.5%, enhancing the active surface area from 33 to 115 m2 g–1, while simultaneously reducing Ru particle size from 18.4 to 3.2 nm. In situ spectroscopy and surface reaction experiments revealed that the CO* pathway occurs for CO2 methanation on both catalysts, which involves CO2 dissociation and subsequent CO* hydrogenation. The smaller Ru nanoparticles on Ru-0.1%Li+/SiO2 exhibit superior intrinsic activity for both steps compared to the larger nanoparticles on Ru/SiO2. The additional alkaline sites introduced by Li+ additives also promote CO2 dissociation. The exceptional activity of Ru-0.1%Li+/SiO2 for CO2 methanation is governed by the synergistic effect between the Ru particle size effect and Li+-induced basicity, with the former being predominant.
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ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Guiming Xie,Xingyang Bai,Yanrui Niu,Runduo Zhang,Jian Liu,Qingyuan Yang,Zhou-Jun Wang
Making use of novel materials to develop efficient catalysts is one of the research hotspots for CO2 hydrogenation to methanol. Herein, UiO-66, a typical Zr-MOF, was modified by ethylene diamine tetraacetic acid (EDTA) to serve as a substrate for the synthesis of AuCu bimetallic catalysts. The resultant AuCu@UiO-66-EDTA catalyst exhibited a superior methanol production rate, which delivered a high space-time yield of methanol (3.34 gMeOH gmetal–1 h–1) at 250 °C and 3.0 MPa. The EDTA modification was found to effectively confine AuCu nanoparticles inside the framework of MOFs, which significantly reduced the metal particle size and enriched the oxygen vacancy concentration. As a consequence, more active sites were generated for methanol synthesis. Moreover, the AuCu@UiO-66-EDTA catalyst yielded more favorable reaction intermediates that could be converted to methanol at a faster rate. This work develops unique MOFs-encapsulated bimetallic catalysts and illuminates the positive effect of confinement.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Yuting Li,Dandan Wang,Yuqin Ma,Fangbin Liu,Hongji Li,Qigming Xu,Haijiao Xie
The reduction of carbon dioxide (CO2) using electrochemical methods is one of the ways to achieve carbon recycling, as the increase in carbon dioxide emissions causes environmental problems. Single-atom dispersed Ni-NC site catalysts have emerged as effective electrocatalysts for the reduction of CO2 to CO. Using ZIF-8 as a carrier, we aim to design a high-performance single nickel-site catalyst by elucidating the structure evolution of NiNx sites during thermal activation as well as other key external factors such as the carbon particle size and nickel content. The pyridine N active sites generated after calcination have higher activity and CO selectivity. The catalyst achieved up to 99.6% CO generation at −0.88 V vs. RHE, and is one of the best catalysts for the reduction of CO2 to CO. This work demonstrates an effective method for designing efficient electrochemical CO2 reduction catalysts by tuning the surface structure of single-atom anchored carriers.
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