ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Yanpeng Chen,Xing Zhu,Kongzhai Li,Yonggang Wei,Yane Zheng,Hua Wang
Syngas generation via thermochemical H2O–CO2 splitting relies heavily on a high-temperature decomposition of metal oxides into a reduced state. Meanwhile, typical chemical looping partial oxidation of methane to syngas suffers from the carbon deposition and the low selectivity toward syngas. To overcome these drawbacks, the partial oxidation of methane and H2O–CO2 splitting are coupled to consist of an alternative chemical looping redox scheme for the generation of Fischer–Tropsch (F–T)-ready syngas. The usability of lattice oxygen in a redox catalyst is facilitated, and its redox property is also thermodynamically optimized by using H2O and CO2 as soft oxidants, guaranteeing an effective generation of syngas from both redox steps. The carbon tolerance is greatly enhanced due to H2O or CO2 gasification in the reoxidization step. Experimental studies confirm the redox scheme by using CeO2–LaFeO3 redox catalyst, demonstrating generation of syngas with an H2/CO molar ratio around 2.0 in both methane partial oxidation and H2O–CO2 splitting steps over 30 repeated cycles at 850 °C. A syngas selectivity of 95% in methane partial oxidation and nearly 100% conversion of CO2 to CO can be achieved. Synergistic effect and competing reaction between H2O and CO2 splittings over the reduced redox catalyst are the key factors for the control of syngas composition and the intensification of CO2 splitting. The proposed approach can potentially be applied for production of F–T-ready syngas with an increased yield without the need for gas separation when compared to the state-of-the-art thermochemical splitting or methane chemical looping partial oxidation processes.
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高影响因子
Advanced Fiber Materials
·
2019
·Vol. 1
·期 3
·222-230
·
IF 0
Liang Liping,Dong Yanyan,Wang Hongfang,Meng Xu
Stimuli-responsive materials with switchable wettability have promising practical applications in oil/water separation. A novel CO 2 -responsive cotton fabric for controlled oil/water separation was fabricated based on mussel-inspired reaction and polymerized with 2-(dimethylamino)ethyl methacrylate (DMAEMA). As expected, the modified fabric exhibited switchable hydrophilicity and hydrophobicity after CO 2 /N 2 alternation, and it could be used for gravity-driven CO 2 -controlled oil/water separation. Water was selectively penetrated through the fabric and separated from oil after treating by CO 2 . A reversed wettability could be generated through simply treated with N 2 . It is expected that the as-prepared fabrics could be applied in smart oil/water separation due to the attractive properties of CO 2 -switchable system.
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Journal of CO2 Utilization
·
2021
·
IF 7.132
Danqing Shu,Miao Wang,Fengyu Tian,Honglei Zhang,Chuang Peng
Electroreduction of CO 2 to high value-added products such as hydrocarbons provides a promising way to create a carbon neutral circular economy. Copper (Cu) is the most effective metal catalyst with selectivity towards hydrocarbons but Cu catalyst alone generally produces hydrocarbons at low selectivity and yield. Operando surface enhanced infrared absorption spectroscopic (SEIRAS) analysis reveals that the low hydrocarbon yield is attributed to the poor ability of Cu to produce carbon monoxide (CO), which is a crucial intermediate for hydrocarbon formation. In the current study, an Ag-Cu dual-cathode CO 2 RR device is developed, which allows separate control of electrode potential. This dual-cathode cell shows increased hydrocarbon yield (83 % for methane and 106 % for ethylene) and a 200 mV lower onset potential for C 2 H 4 , compared to electrolysis with a single Cu cathode. The CO produced by the Ag cathode transfers to Cu and increase its CO coverage, facilitating methane formation as well as promoting C C coupling to form ethylene. This study also reveals a mismatch of optimum electrode potential between Ag and Cu, which results in compromised performance of the two components in an Ag-Cu bimetallic electrocatalyst, but poses no challenge in the dual-cathode cell. To optimize the performance of the dual-cathode cell, we propose the use of a single-pass dual-gas-diffusion-cathode reactor with enhanced mass transfer for maximum hydrocarbon production. This work verifies that splitting the complex CO 2 RR process into two separate steps is a feasible method to improve the overall efficiency and rate of advanced products while reducing the energy input.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2019
·Vol. 30
·期 8
·7950-7962
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IF 2.195
Hu Bingbing,Guo Qiang,Wang Kang,Wang Xitao
In this paper, a series of indium oxides were prepared by calcining the In(OH) 3 precursors, which were synthesized by hydrothermal method using the mixed solution of ethylenediamine (En) and water as a solvent. The morphologies, particle sizes, pore structure, crystallinity and surface defect concentration of these photocatalysts were adjusted by varying the ratio of En to water during the preparation of In(OH) 3 precursors. The results revealed that In 2 O 3 photocatalysts obtained from the precursor prepared in En containing solvent exhibited much higher photocatalytic activities for CO 2 reduction with H 2 O when compared to that derived from the precursor prepared in pure water. This result can be ascribed to several reasons as following. Firstly, the En addition with a suitable amount can improve the crystallinity of In 2 O 3 and decrease the surface defect concentration, which obviously depressed the recombination of photogenerated electrons and holes. Also, the addition of En during the preparation of precursor can decrease the particle size, increase specific surface area and pore structure, resulting into the increase of active sites. Finally, the band gap of In 2 O 3 can be slightly narrowed after the addition of En, resulting in enhanced light absorption in the visible region. When the ratio of ethylenediamine to water is 1:1, the as-prepared In 2 O 3 possessing the largest specific surface area and pore volume, enhanced light absorption ability and higher hole–electron separation efficiency, exhibited the highest photocatalytic activity. Under visible light irradiation, the H 2 , CO and CH 4 production rates of 5.3, 8.3 and 27.2 µmol/g cat /h can be achieved, respectively.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shuyi Xia,Xiang Wang,Deqi Fan,Yingying Li,Yi Lu
Freshwater scarcity and rising atmospheric CO 2 are two pressing environmental challenges. Here we report a multifunctional electrospun bilayer nanofibrous membrane that integrates solar-driven interfacial water evaporation with photocatalytic CO 2 reduction in a single platform. The top PAN/CNT layer delivers broadband solar absorption and efficient photothermal conversion, while the bottom CoAl-LDH/PAN layer provides catalytic sites and capillary-assisted water transport, stabilizing a three-phase reaction interface. Under one-sun illumination, the bilayer nanofibrous membrane achieves a water evaporation rate of 2.5 kg·m −2 ·h −1 and the CAL/PAN-6 % layer within it delivers a CO evolution rate of 287.6 μmol·g −1 , both outperforming single-layer counterparts. Spectroscopic and electrochemical analyses reveal suppressed charge recombination and enhanced carrier lifetimes, and outdoor tests confirm robust operation under fluctuating sunlight. The solvent-based but recyclable electrospun architecture presents a scalable environmental materials platform that couples clean water supply with carbon mitigation, offering a viable route toward sustainable water-energy-carbon integration.
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Molecular Catalysis
·
2025
·
IF 4.9
Meilin Yin,Jingchen Li,Simai Peng,Daying Chen
The industrial implementation of CO 2 cycloaddition remains hindered by catalysts that require multi-step syntheses, co-catalysts or solvents, and yet offer limited recyclability and scalability. Here, we present a metal-free heterogeneous composite catalyst (PImBr@COF) prepared by a 6 h one-pot ship-in-bottle polymerization of imidazolium ionic liquids within the ordered nanochannels of an imine-linked triazine COF (HO-TAPT-COF). This strategy simultaneously embeds Br – nucleophiles, hydrogen-bond donors (-OH) and CO 2 -philic moieties (imine, triazine groups and imidazolium cations) into a crystalline porous scaffold, creating a cooperative activation environment for epoxide ring-opening and CO 2 coupling. The resulting catalyst achieves a CO 2 /N 2 selectivity boost from 14.2 to 24.7, maintains a CO 2 uptake of 50.6 mg g −1 , and delivers a 99.0 % yield of cyclochloroallyl carbonate under solvent- and cocatalyst-free conditions. Remarkably, both CO 2 capture and catalytic activity show negligible decay after ten cycles. Density functional theory calculations reveal that the confined ionic environment significantly lowers the energy barrier for epoxide activation. This work establishes a rapid, scalable and broadly applicable route for constructing multifunctional COF-based catalysts for sustainable CO 2 utilization.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2016
·
IF 2.196
Yong-Jie Geng,Jie Wang,Zhi-Hong Liu
Two transition metal borates with microporous structures for Na 2 Co 2 B 12 O 21 and Na 2 Cu 2 B 12 O 21 have been synthesized and characterized by XRD, FT-IR, and elemental analysis. The molar enthalpies of solution of Na 2 Co 2 B 12 O 21 (s) and Na 2 Cu 2 B 12 O 21 (s) in 1 mol dm −3 HCl(aq) were measured by microcalorimeter at T = 298.15 K, respectively. The molar enthalpies of solution of CoCl 2 ·6H 2 O(s) and CuCl 2 ·2H 2 O(s) in the mixture solvent of 2.00 cm 3 of 1 mol dm −3 HCl(aq) in which 5.30 mg of H 3 BO 3 and 0.84 mg of NaCl being added were also measured, respectively. With the incorporation of the previously determined enthalpy of solution of H 3 BO 3 (s) in 1 mol dm −3 HCl(aq), together with the standard molar enthalpies of formation for CoCl 2 ·6H 2 O(s)/CuCl 2 ·2H 2 O(s), NaCl(s), H 3 BO 3 (s), HCl(aq) and H 2 O(l), the standard molar enthalpies of formation of – (9072.4 ± 9.7) kJ mol −1 for Na 2 Co 2 B 12 O 21 (s) and – (8887.5 ± 9.7) kJ mol −1 for Na 2 Cu 2 B 12 O 21 (s) at T = 298.15 K were obtained on the basis of the appropriate thermochemical cycles. It is obvious that Na 2 Co 2 B 12 O 21 (s) is more thermal stable than that of Na 2 Cu 2 B 12 O 21 (s).
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiale Wang,Shiyan Ma,Yun Huang,Ao Xia,Xianqing Zhu,Xun Zhu,Qiang Liao
Microalgae, as efficient photosynthetic autotrophs, hold significant potential for carbon sequestration. However, their photosynthesis is constrained by the selective use of the solar spectrum. To enhance the utilization of natural light energy, a dual functional substrate with ultraviolet (UV) light conversion and microalgae biofilm support was proposed by coating a rare earth complexes phosphor agent onto transparent acrylic in this study. By doing this, UV light could directly drive microalgae biofilm photosynthesis by converting it to red light, resulting in a maximum 2.81 times increase in the carbon fixation rate. The UV conversion substrate increased the electron transport rate of microalgal photosystem II by 58.08%, effectively enhancing the photosynthetic rate and oxygen release, promoting the formation of a porous biofilm structure, and strengthening the material transfer within the biofilm. Additionally, reactive oxygen species (ROS) can cause oxidative stress, affecting cell growth and metabolic activity. With the use of the UV conversion substrate, the levels of ROS and malondialdehyde (MDA) in microalgae decreased by 84.56% and 42.35%, respectively. Consequently, UV-induced damage to microalgae cells was reduced, leading to a 52.52% increase in the photosynthesis rate and achieving UV driven photosynthetic carbon sequestration. This study demonstrated the UV conversion substrate’s effectiveness in reducing UV-induced damage in microalgae and enhancing photosystem activity, showing significant potential for carbon fixation within microalgal biofilms.
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RSC Advances
·
2024
·Vol. 14
·期 29
·21151-21157
·
IF 3.9
Jianwei Yang,Xianghao Han,Xiao Feng
As an emerging category of crystalline porous materials, covalent organic frameworks (COFs) are primarily synthesized via solvothermal methods. However, achieving rapid synthesis of COFs through this approach poses a significant challenge. To address the issue of slow synthesis, we studied the crystallization process of aminal-linked COFs via the condensation of a cost-effective aldehyde and secondary amine, and successfully expedited the synthesis of COFs within a one-hour duration. Furthermore, gram-scale aminal-linked COFs with abundant ultra-microporous channels demonstrated promising potential for CO2/CH4 separation. This study enables the rapid synthesis of aminal-linked COFs from cheap raw materials, which lays a foundation for their practical applications.
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PubMed
高影响因子
Nano Energy
·
2025
·
IF 17.1
Peng Bai,Jiafa Chen,Yicheng Zhao,Yongdan Li
CO 2 formylation of amines provides a promising route to convert CO 2 into value-added chemicals. That process is usually performed through a thermo-catalytic approach with additional reducing agents, which increases the energy consumption and the complexity of the system. Herein, we report photocatalytic CO 2 formylation of benzylamine over Pt 1 In-ZnO x single-atom-alloy catalyst at room temperature in N , N -dimethylformamide (DMF) solvent. The anchoring of Pt single atoms onto In nanoparticles through Pt-In bonds accompanied with electron transfer from In to Pt improves the absorption capacity for visible light and the separation efficiency of photogenerated charge carriers. Furthermore, the adsorption and activation of CO 2 and benzylamine are promoted on the surface of Pt 1 In single-atom-alloy. After 6 h reaction under visible-light, the yield of N -benzylformamide reaches 48.6 mmol g −1 with a 95.3 % selectivity. A possible reaction mechanism is proposed based on a series of in situ characterizations and theoretical calculations. A decomposition-regeneration cycle of DMF is involved in the photocatalytic process, which extends the reaction region and thus facilitates the formylation of benzylamine. The photocatalytic system exhibits good cycling stability and universality. This work provides new insights for the rational design of single-atom-alloy catalyst and an efficient approach for the sustainable utilization of CO 2 .
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Yingzi Hu,Yan Zhu,Xi He,Ya-Nan Feng,Fei-Fei Chen,Yan Yu
Two-dimension nanosheets are ideal photocatalysts for CO 2 reduction due to their high exposure of active sites and short charge transfer pathway. However, 2D photocatalysts have a tendency to agglomeration, thus compromising the performance of photocatalytic CO 2 reduction. Trees, one of the most important plants for photosynthesis, have a unique “leaf-on-branch” structure. This unique two-dimension/one-dimension (2D/1D) configuration maximizes the adsorption of CO 2 molecules and light harvesting. Herein, a tree-inspired semiconductor-on-ceramic 2D/1D heterostructure for efficient photocatalytic CO 2 reduction is reported. The cobalt silicate (CoSi) nanosheets (∼0.68 nm) are in situ grown on the surfaces of hydroxyapatite (HAP) nanowires, creating a well-defined 2D/1D hierarchical structure. The vertical alignment of ultrathin CoSi nanosheets on the HAP nanowires effectively suppresses their agglomeration, leading to a large BET surface area (106.45 m 2 /g) and excellent CO 2 adsorption (8.00 cm 3 g −1 ). The results of photoelectrochemical characterization demonstrate that the 2D/1D hierarchical structure is powerful to expedite charge transfer. As a result, the gas generation rate of CO is as high as 28780 μmol g −1 h −1 over the CoSi-on-HAP 2D/1D heterostructure. In addition, the electron transfer mechanism and reaction pathways of CO 2 reduction are revealed by in situ irradiated XPS and in situ DRIFT spectra.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fayi Jin,Xiaoli Yang,Jia Yang,Yang Lei,Wenfan Xu,Wei Jiang,Zhen Ma,Gemeng Liang,Haoxi Ben,Xingyun Li
Oxygen vacancies in oxides are core parameters determining the catalytic performance in various reactions. This study investigated the influence of oxygen vacancies of MoO x catalysts on the reverse water gas shift (RWGS) reaction to gain a deep insight into the structure–function relationship. A distinct volcano-shaped trend was observed among MoO x catalysts with different amounts of oxygen vacancies. Through comprehensive characterizations and steady-state kinetic analysis, an optimal concentration of oxygen vacancies was identified to not only facilitate the adsorption and activation of CO 2 but also restrain the formation of by-product CH 4 . In-situ characterizations combined with DFT calculations uncovered a formate-involved reaction pathway over the oxygen vacancies structured MoO x catalyst, with the hydrogenation of formate identified as the rate-determining step. These findings not only showcase the potential of Mo-based oxides in CO 2 hydrogenation reactions but also provide fundamental insights into the role of oxygen vacancies in shaping catalytic behavior.
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