CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Qi Liu,Tong Luo,Yiyan Yin,Yan Ouyang,Min Xiao,Hongxia Gao,Teerawat Sema,Zhiwu Liang
Amine degradation is one of the key issues that hampers the implementation of amine-based post combustion carbon capture technology. In this work, the oxidative degradation of fourteen structurally varied amines were experimentally studied by measuring the amine loss, alkalinity change, ammonia yield, and degradation product. There is a linear relationship between amine loss against alkalinity change and ammonia yield, indicating that the degradation product either loss reactivity for CO 2 absorption or emit out as the small molecule. The results have shown that amine stability generally increased with amine order and stronger steric hindrance effect. Most primary and secondary amines showed more than 40 % amine loss after 336 h degradation experiment, while most of tertiary amines showed less than 10 % amine loss. This may be due to the exposed amine groups of primary and secondary amines. The oxidative degradation mechanism was studied based on density functional theory (DFT) calculations.
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Small
·
2024
·Vol. 20
·期 31
·2310894
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IF 13
Jie Chen,Yang Liu,Quanhua Xie,Yuanyuan He,Dengjie Zhong,Haixing Chang,Shih-Hsin Ho,Nianbing Zhong
A visible-light-driven CO 2 reduction optical fiber is fabricated using graphene-like nitrogen-doped composites and hollow quartz optical fibers to achieve enhanced activity, selectivity, and light utilization for CO 2 photoreduction. The composites are synthesized from a lead-based metal–organic framework (TMOF-10-NH 2 ) and g-C 3 N 4 nanosheet (CNNS) via electrostatic self-assembly. The TMOF-10-NH 2 /g-C 3 N 4 (TMOF/CNNS) photocatalyst with an S-type heterojunction is coated on optical fiber. The TMOF/CNNS coating, which has a bandgap energy of 2.15 eV, has good photoinduced capability at the coating interfaces, high photogenerated electron–hole pair yield, and high charge transfer rate. The conduction band potential of the TMOF/CNNS coating is more negative than that for CO 2 reduction. Moreover, TMOF facilitates the CO desorption on its surface, thereby improving the selectivity for CO production. High CO 2 photoreduction and selectivity for CO production is demonstrated by the TMOF/CNNS-coated optical fiber with the cladding/core diameter of 2000/1000 µm, 10 wt% TMOF in CNNS, coating thickness of 25 µm, initial CO 2 concentration of 90 vol%, and relative humidity of 88% RH under the excitation wavelength of 380–780 nm. Overall, the photocatalytic hollow optical fiber developed herein provides an effective and efficient approach for the enhancement of light utilization efficiency of photocatalysts and selective CO 2 reduction.
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ChemistrySelect
·
2024
·Vol. 9
·期 44
·e202403927
·
IF 1.9
Hui Han,He Cui,Jiabo Wang,Kai Ge,Yongfang Yang
Graphical In this paper, 2D MOF-Co, 2D MOF-Co/Cu, and 2D MOF-Co/Cu/Fe are designed and prepared using 1,4-benzendicarboxylic acid (1,4-BDC) as organic ligands. Their charge transfer, separation efficiency, and effects on photocatalytic CO 2 reduction are studied. The results show that 2D multimetallic MOF-Co/Cu/Fe has better photocatalytic CO 2 reduction activity, so it has higher research value and development prospect in the field of photocatalytic CO 2 reduction. In this study, 2D multimetallic MOFs combined with the advantages of 2D nanosheets, with the synergetic effect of multimetallic nodes, exhibited good photocatalytic activity for reduction of CO 2 . Herein, a 2D MOF-Co/Cu/Fe were successfully prepared via one-pot stirring of the solutions of multimetal salts and organic ligands at room temperature. Introduction of the second and third metal (Cu and Fe) into MOF-Co does not change the 2D morphology of MOFs, although it improved the photocatalytic CO 2 reduction performance by broadening the light absorption range of 2D MOF-Co, accelerating the separation efficiency and transfer rate of photogenerated carriers. Upon irradiation with full-spectrum light, the average CO yield of 2D MOF-Co/Cu/Fe achieved 17.06 µmol·g −1 ·h −1 , being about 1.8 and 1.2 times that of 2D MOF-Co and 2D MOF-Co/Cu. This work provides an insight into 2D multimetallic MOFs-based photocatalysts in catalytic CO 2 reduction.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Hongyu Ma,Xi Wu,Xinghua Li,Jie Liu,Haipeng Dong,Yu Liu,Luyao Niu,Fang Zhang,Wenbo Wang,Changlu Shao,Xiaowei Li,Yichun Liu
Photocatalytic carbon dioxide (CO2) reduction for high-value hydrocarbon fuel production is a promising strategy to tackle global energy demand and climate change. However, this technology faces formidable challenges, primarily stemming from low yield and poor selectivity of C2 products of the desired hydrocarbon fuels. This study reported ZnO/ZnCo2O4 Janus hollow nanofibers (ZnO/ZCO JHNFs) prepared by electrospinning and atomic layer deposition. Photocatalytic tests revealed an ethanol yield of 4.99 μmol g–1 h–1 for ZnO/ZnCo2O4 JHNFs, surpassing mixed ZnO/ZnCo2O4 nanofibers (ZnO/ZCO NFs) by 4.35 times and pure ZnO by 12.7 times. The selectivity of 58.8% is 2.38 and 4.49 times higher than those of ZnO/ZnCo2O4 NFs and ZnO, respectively. These enhancements are attributed to efficient carrier separation facilitated by the ordered internal electric field of the Z-scheme heterojunction interface, validated by the energy band evaluations from experimentation and density functional theory (DFT) simulations and charge separation characterizations of photocurrent, impedance, and photoluminescence spectra. The Janus structure also effectively exposes the surface of ZnCo2O4 to CO2 molecules, increasing the active site availability, as confirmed by BET nitrogen adsorption/desorption, temperature-programmed desorption tests, and DFT adsorption energy calculations. This study proposes a novel approach for efficient photocatalytic hydrocarbon fuel production, with potential applications in energy and climate crisis mitigation.
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ACTA PHYSICO-CHIMICA SINICA
·
2025
·
IF 13.5
Qinhui Guan,Yuhao Guo,Na Li,Jing Li,Tingjiang Yan
In the realm of photocatalytic CO 2 hydrogenation, the adsorption-desorption behaviors and dynamics of photogenerated carriers are pivotal determinants of the kinetic processes and overall efficiency of photocatalytic reactions. Herein, 5A molecular sieve-functionalized In 2 O 3 composites (denoted as IO@5A- x wt%) were fabricated through a facile impregnation-calcination method. Among them, the IO@5A-5wt% composite, with the optimized loading amount of 5A molecular sieves, showcases outstanding performance in photocatalytic conversion of CO 2 to CO, achieving a CO production rate of 2610.55 μmol·g −1 ·h −1 , which is 19 times higher than that of pristine In 2 O 3 . Moreover, the IO@5A-5wt% composite maintains acceptable catalytic stability after a prolonged experiment lasting 45 hours and total of 108 cycles. A comprehensive series of characterization techniques and performance evaluations reveal that the incorporation of 5A molecular sieves significantly modulates the adsorption-desorption behavior and hole dynamics during photocatalytic reactions. The multi-channel architecture of 5A molecular sieves, featuring suitable pore sizes, effectively enhances CO 2 adsorption. Meanwhile, the surface hydroxyl groups of 5A molecular sieves facilitate the transfer of photogenerated holes, thereby suppressing the recombination of photogenerated carriers. Additionally, the reaction product H 2 O desorbs more readily from the catalyst surface. These synergistic effects collectively constitute the key mechanism underlying the enhanced photocatalytic performance of the IO@5A-5wt% composite.
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ACS Nano
·
2024
·
IF 15.8
Xue Tian,Huan Liu,Bin Cao,Peng Zhang,Yanze Li,Yanchao Ou,Haonan Cui,Mengyao Xu,Bin Xu
MXenes are promising cathodes for Li–CO2 batteries owing to their high electrical conductivity and efficient CO2 activation function. However, the effects of adsorption and electronic structures of MXene on the full life cycle of Li–CO2 batteries have been rarely investigated. Here, we employ a coregulation approach to enhance the adsorption–decomposition of lithium carbonate (Li2CO3) by introducing Zn and Cl surface groups onto the Ti3C2 MXene (Zn–Ti3C2Cl2) catalyst. The incorporation of Cl surface groups enhances Li2CO3 adsorption on the MXene catalyst surface, resulting in the formation of small-sized and uniform Li2CO3. Additionally, the introduction of Zn shifts the d-band centers of titanium and promotes CO2 evolution reaction (CO2ER) activity, thereby facilitating the decomposition of discharge products. As a result, the Li–CO2 battery based on the Zn–Ti3C2Cl2 catalyst exhibits an ultralow overpotential (0.72 V) at 200 mA g–1 and stable cycling for up to 1500 h. This work validates the efficacy of promoting reversibility in Li–CO2 batteries by adjusting the adsorption-decomposition process.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Yuchun Liu,Tianqi Liu,Xinyun Wang,Jing Zhang,Xingwu Zhai,Tianchen Wei,Qianqi Shi,Chengjie Lu,Huan Yan,Yujian Xia,Weiren Cheng,Min Zhou
Li-CO₂ batteries promise ultrahigh theoretical energy densities but face efficiency limitations owing to the sluggish decomposition of stable Li 2 CO 3 . Redirecting the redox pathway toward Li 2 C 2 O 4 overcomes this challenge, but its metastability leads to facile conversion to Li 2 CO 3 during discharge. Herein, subsurface electronic confinement is engineered in Mo-based catalysts, leveraging electron-deficient boron (B) as electron traps in the subsurface atomic layers to tailor their interfacial electronic landscapes. This design elevates the Mo d-band and intensifies the hybridization between the Mo d-orbitals and O p-orbitals of oxalate. Strengthening the Mo-O interaction stabilizes Li 2 C 2 O 4 against decomposition. The highly reversible and stable redox chemistry enabled by MoB results in an exceptional cycling stability and energy efficiency across a wide temperature range, with an expanded practical viability. At 70 µA cm −2 , the MoB-based battery is cycled for >1400 h with a high energy efficiency of >85%. The energy efficiency even remains at >90% for ≈150 h at a high temperature (90 °C). This study pioneers a material design framework for use in stabilizing metastable products within Li-CO 2 batteries, advancing their applicabilities in extreme environments, such as deep-earth exploration, by revealing the role of subsurface charge redistribution in steering reaction pathways.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Shuai Yan,Yuting Wang,Guangyao Chen,Wanli Ma,Yingquan Chen,Xianhua Wang,Kuo Zeng,Yonggang Yao,Hongqi Sun,Haiping Yang,Hanping Chen
Transition metals doping for Fe-based catalysts has been demonstrated in promoting the activity and regulating the selectivity in both reverse water gas shift reaction and Fischer-Tropsch synthesis. However, there are few studies that concern their catalytic performances tailored by these promoters under photothermal conditions. In this study, a series of typical MFeOx (M = Mn, Co, Cu, Zn) catalysts were synthesized with a facile co-precipitation method and their photothermal CO2 hydrogenation properties were evaluated. The results showed that the doping of Co, Cu, and Zn enhanced the activity and regulated the selectivity of Fe-based catalysts, e.g., CoFe achieving a C2+ yield of 1.73 mmol·h-1·g-1 while ZnFe almost doubling the CO2 conversion under irradiations. Mechanistic studies suggest that Co and Cu facilitated the reduction of Fe species, resulting in favorable CO2 and H2 activation. At last, a light-induced direct CO2 dissociation pathway was proposed with in situ EPR and DRIFTS characterization and analysis of the undoped Fe and ZnFe catalyst. This study provides a novel perspective on transition metal promoters for photothermal CO2 hydrogenation over Fe-based catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Minglu Li,Siyu Kuang,Yaxin Jin,Haoyuan Chi,Sheng Zhang,Xinbin Ma
Copper-based catalysts exhibit an excellent ability in producing C 2 chemicals during CO 2 RR. However, the unsustainable Faradic efficiency (FE) resulting from the reconstruction makes keeping catalyst behavior challengeable. In this study, we synthesized CuO nanosheets and incorporated a small amount of nickel on surface to improve the stability of nanosheets. By inhibiting the dissolution of Cu through the incorporation of Ni, our CuO + Ni-surface catalyst could achieve a double increase in stability compared to CuO nanosheets. Using a combination of electrochemistry, density functional theory calculations, in situ UV–vis spectrometer and inductively coupled plasma optical emission spectrometry, we elucidate the mechanisms behind the increased stability. The incorporation of Ni reduces the tendency of Cu oxidation at higher overpotential and strengthens the bonds between surface and subsurface Cu atoms. This work highlights a promising approach to enhance the stability and efficiency of copper-based catalysts in CO 2 RR, proposing the way for more sustainable catalytic processes.
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ACS Omega
·
2024
·
IF 3.7
Liyuan Cai,Jingchun Wu,Miaoxin Zhang,Keliang Wang,Zhao Yang
Phase separation of microemulsions occupies a key position in many applications, such as oil recovery, nanomaterial synthesis, and chemical reactions. Achieving an intelligent response is crucial to microemulsion development and application. For this reason, in this study, CO2-responsive superamphiphilic molecules were developed as rapidly switchable oil-in-water microemulsions. These superhydrophilic molecules with linear structures were produced by electrostatic interaction of stearic acid and aminotrimethyltriazine COSM-1 in a 1:1 molar ratio. The introduction of n-butanol as a cosurfactant in the CO2-responsive microemulsion system resulted in the spontaneous formation of stable microemulsions. The effect of the addition of n-butanol on the carbon dioxide-responsive microemulsion system was investigated, and the optimum amount of n-butanol was determined by optimization. After exposure to CO2 for 30 s, the superhydrophilic molecules decomposed into inactive components at the interface, leading to a complete phase separation of the microemulsion into oil and water phases. The system was purged with N2 at 60 °C for 10 min to remove the CO2, and the phase separation system was transformed into a clear microemulsion, which was then evaluated for its properties. The rapid response and complete demulsification of these surface CNFS superamphiphiles to CO2 suggest that they have promising applications in product separation, microemulsion recovery, and enhanced crude oil recovery.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Weida Chen,Meisi Chen,Bin Jiang,Tong Lei,Feng Zhang,Zhibing Zhang
Biphasic absorbents composed of tetraethylenepentamine, 1-ethylimidazole, and H 2 O (TEH) exhibit notable absorption rates and CO 2 loads. However, troublesome precipitation forms in the enriched phase due to strong interactions among absorption products. To address this issue, six amino acid ionic liquids (AAILs) were introduced as split-phase regulators in TEH, developing a liquid–liquid biphasic absorption system TEH-AAILs, with outstanding absorption performance. By analyzing the kinetic data and establishing the evaluation parameters, combined with molecular dynamics simulations, the effects of AAILs on the loading and phasing performance were assessed. Remarkably, TEH-[Ser] was screened to possess good performance. Spectral analysis of the TEH-[Ser] reaction mechanism further elucidates the bridged hydrogen bonding structure between [Ser]–CO 2 and H 2 O, highlighting its role in enhancing regeneration efficiency. This study provides insights into the design and optimization of biphasic absorbents for efficient CO 2 capture.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Weida Chen,Meisi Chen,Tong Lei,Feng Zhang,Jiao Geng
High regeneration energy is a critical barrier to the large-scale implementation of CO2 capture technologies. To address this challenge, we present a novel energy-efficient biphasic absorbent system, designed by incorporating sterically hindered amine ionic liquids (AMP-TZ) with N,N,N′,N′-tetramethyl-1,6-hexanediamine (TMHDA). The innovative design focuses on enhancing the spatial site resistivity of ionic liquids, which plays a key role in optimizing the CO2 absorption and minimizing regeneration energy. This system demonstrates superior performance, achieving a CO2 absorption capacity of 2.72 mol/kg at 313.2 K and 150 kPa, with a low regeneration energy of 2.31 GJ/t of CO2. Molecular dynamics simulations and quantum chemical calculations reveal that AMP-TZ promotes proton transfer during absorption and stabilizes bicarbonate (HCO3–) in the CO2-rich phase via weak hydrogen bonding. The unique role of AMP-TZ as a bifunctional hydrogen bond donor/acceptor and its ability to suppress the self-aggregation of HCO3– enhance both the absorption efficiency and regeneration performance. This study provides insights into the design of low-hydration CO2 capture systems and offers a theoretical framework for developing highly efficient, energy-saving biphasic absorbents.
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