Small
·
2023
·
IF 13.3
Kai Zhang,Cuiping Xu,Xingjian Zhang,Zhiyi Huang,Qixiang Pian,Kunhong Che,Xiaokun Cui,Yueru Hu,Yimin Xuan
The chemical inertness of CO 2 molecules makes their adsorption and activation on a catalyst surface one of the key challenges in recycling CO 2 into chemical fuels. However, the traditional template synthesis and chemical modification strategies used to tackle this problem face severe structural collapse and modifier deactivation issues during the often-needed post-processing procedure. Herein, a CO 2 self-selective hydrothermal growth strategy is proposed for the synthesis of CeO 2 octahedral nanocrystals that participate in strong physicochemical interactions with CO 2 molecules. The intense affinity for CO 2 molecules persists during successive high-temperature treatments required for Ni deposition. This demonstrates the excellent structural heredity of the CO 2 self-selective CeO 2 nanocrystals, which leads to an outstanding photothermal CH 4 productivity exceeding 9 mmol h -1 m cat -2 and an impressive selectivity of >99%. The excellent performance is correlated with the abundant oxygen vacancies and hydroxyl species on the CeO 2 surface, which create many frustrated Lewis-pair active sites, and the strong interaction between Ni and CeO 2 that promotes the dissociation of H 2 molecules and the spillover of H atoms, thereby greatly benefitting the photothermal CO 2 methanation reaction. This self-selective hydrothermal growth strategy represents a new pathway for the development of effective catalysts for targeted chemical reactions.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Huijie Wang,Jiaye Zhu,Xuhui Ren,Yun Tong,Pengzuo Chen
Tuning coordination environment of single-atom catalysts (SACs) is widely applied for the electrochemical CO 2 reduction reaction (CO 2 RR). However, the influence of the interaction between SACs and support on the catalytic performance are not comprehensive. Herein, taking cobalt phthalocyanine (CoPc) as a conceptual example, a hetero S-atom doping strategy of hollow carbon sphere (S-NHC) is put forward as a carrier, revealing the intrinsic relationship between microenvironment regulation and catalytic activity of single Co-atom. The additional S doping may induce more carbon defect and increases the content of pyrrolic N in the S-NHC sample, leading to stronger electronic interaction of heterogeneous CoPc/S-NHC for boosting CO 2 RR performance. Remarkably, the catalyst achieves a highest CO selectivity of nearly 100% at −0.6 V, and the FE CO are over 90% in a wide potential range from −0.4 to −0.8 V in a flow cell. The maximum power density is high as 2.68 mW cm −2 at 4.7 mA cm −2 for the Zn–CO 2 battery with CoPc/S-NHC cathode. In situ attenuated total reflection infrared (ATR-IR) spectroscopy reveals the formation of key *COOH and *CO intermediates, while the calculation result confirm the optimized Gibbs free energy of these intermediates on CoPc/S-NHC, suggesting the feasibility of the regulation strategy.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 24
·9725-9731
·
IF 3.069
Suresh Mutyala,Sobhy M. Yakout,Shebl S. Ibrahim,Madhavi Jonnalagadda,Harisekhar Mitta
Iron metal–organic framework, MIL-100(Fe) was prepared by a hydrothermal method and used as a support to incorporate diethylenetriamine (DETA) for the study of CO2 adsorption and separation of CO2/N2. All synthesized adsorbents were characterized by PXRD, N2 adsorption–desorption isotherms, FT-IR, TGA, SEM, and elemental analysis. Structural characterization results have revealed that the structure of MIL-100(Fe) was not changed by the incorporation of diethylenetriamine. The CO2 adsorption capacities were 29 cm3 g−1 and 41 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. Adsorption of CO2 on DETA–MIL-100(Fe) was higher than that on MIL-100(Fe). The enhancement was due to the presence of amine groups which could form ammonium carbamate by interaction with CO2. Similarly, the N2 adsorption capacities were 3 cm3 g−1 and 0.9 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. The decrease in N2 adsorption capacity was due to the decrease in surface area. The selectivity of CO2/N2 on DETA–MIL-100(Fe) was four times higher than that on MIL-100(Fe). The heat of CO2 adsorption was 74.2 kJ mol−1 at low coverage of CO2 on DETA–MIL-100(Fe) and the CO2 adsorption capacity was constant in each adsorption cycle over the same adsorbent.
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CHINESE CHEMICAL LETTERS
·
2014
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IF 1.178
Wei Wang,Ye Yuan,Fu-Xing Sun,Guang-Shan Zhu
Novel porous aromatic frameworks (PAF-53 and PAF-54) have been obtained by the polymerization of amino compound ( p -phenylenediamine and melamine) and cyanuric chloride. They display a certain amount of CO 2 adsorption capacity and highly selective separation of CO 2 /CH 4 and CO 2 /N 2 as 18.1 and 83 by Henry Law respectively. They may be applied as ideal adsorbents to separate and capture CO 2 .
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FLUID PHASE EQUILIBRIA
·
2015
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IF 2.2
Shufeng Shen,Ya-nan Yang,Yong Wang,Shaofeng Ren,Jiangze Han,Aibing Chen
Amino acid salts have potential use as alternative absorbents to alkanolamines for post combustion CO 2 capture, because of their negligible volatility, resistance to oxidative degradation and fast absorption rates. In this work, the density and viscosity of CO 2 -free and CO 2 -loaded aqueous solutions of potassium lysinate (LysK) and potassium prolinate (ProK) were measured at temperatures from (298.15 to 348.15) K and for their concentrations from (0.2 to 3.0) mol L −1 . The data were correlated accurately ( R 2 ≥ 0.99) as a function of temperature, concentration and CO 2 loading by nonlinear regression analysis. The solubility of CO 2 in 2.5 mol L −1 amino acid salt solutions was also determined in vapor–liquid equilibrium vessels at temperatures (313 and 333) K and CO 2 partial pressures relevant to flue gas conditions. It was found that, the CO 2 absorption capacity of LysK is higher than that of industrially used monoethanolamine (MEA) and the CO 2 loadings vary as LysK > ProK > MEA at given CO 2 partial pressures. Moreover, LysK may offer higher cyclic loading than MEA for CO 2 capture.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Qi Gao,Bo Wang,Japan Trivedi,Xingguang Xu,Shuai Liu
CO2-responsive foam (CRF) is a highly promising candidate for CO2-enhanced oil recovery (CO2-EOR) because it displays higher stability than the surfactant-stabilized foam owing to the formation of robust wormlike micelles (WLMs) upon exposure to CO2. In this work, the nanoparticle-enhanced CO2-responsive foam (NECRF) was properly prepared using lauryl ether sulfate sodium (LES)/diethylenetriamine/nano-SiO2, and its interfacial properties and EOR potential were experimentally and numerically assessed, aiming to explore the feasibility and effectiveness of NECRF as a novel CO2-EOR technique. It was found that the interfacial expansion elastic modulus increased 6-fold after CO2 stimulation. The modulus continued to increase with the introduction of nano-SiO2 owing to the pronounced synergistic effect of WLMs and nanoparticles. In addition to increasing the viscosity of the foaming liquid, WLMs and nano-SiO2 enhanced the shearing resistance of the NECRF as well. Calculations demonstrated that both the coarsening rate and the size distribution uniformity coefficient of NECRF were markedly lower than that of the LES foam, which subsequently inhibited NECRF decay and greatly improved its dynamic stability. Besides, molecular dynamics simulation revealed that adding inorganic salts to NECRF could notably enhance the foaming performance due to the intensified hydration of surfactant head groups and reduced binding energy of neighboring molecules. Nuclear magnetic resonance-assisted core flooding experiments validated the exceptional capacity of NECRF to sweep the low-permeability region and improve the conformance profile. Overall, these findings may provide valuable insights into the development and application of novel materials and strategies for the CO2-EOR.
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Catalysts
·
2025
·Vol. 15
·期 1
·94
·
IF 4
Fuhai Zhang,Jing Xiong,Xiaoxiao Yu,Lei Wang,Tongyu Wu,Zhendong Yu,Minmeng Tang,Haiyan Liu,Yanhong Chao,Wenshuai Zhu
As a promising member of the carbon nitride family, nitrogen-rich g-C3N5has attracted significant attention because of its excellent light absorption performance. Nevertheless, its practical application in photocatalytic CO2reduction is hindered by severe photogenerated charge recombination and limited CO2adsorption capacity. Constructing a heterojunction has emerged as an effective strategy to mitigate charge recombination, thereby enhancing the photocatalytic performance of the catalyst. Herein, a series of CdS/g-C3N5-X heterojunction catalysts were prepared via an in situ hydrothermal approach. The obtained heterojunction catalysts exhibited a novel coral reef-like morphology which facilitated the exposure of additional active sites, thereby enhancing the adsorption and activation of CO2. Moreover, studies have shown that CdS can be anchored to the surface of g-C3N5through C-S bonds, forming a built-in electric field at the interface, which accelerated the separation and transfer of photogenerated charges. Consequently, the resulting heterojunction materials demonstrated high efficiency in photocatalytic CO2reduction with H2O as a sacrificial agent. In particular, CdS/g-C3N5-0.2 exhibited the maximum photocatalytic performance up to 22.9 μmol·g−1·h−1, which was 6 times and 3 times that of unmodified g-C3N5and CdS, respectively. The results indicated that the increased active sites and enhanced charge separation of the Cd/g-C3N5-0.2 catalyst were the primary reasons for its improved photocatalytic CO2reduction performance. This work provides a novel heterojunction-based photocatalyst for efficient CO2photocatalytic reduction, offering insights into the preparation of high-performance photocatalysts for sustainable energy applications.
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ACS Nano
·
2025
·
IF 16
Tonghui Jin,Sophally Chhong,Mingqin Li,Jiangtao Zhou,Qize Xuan,Jiaqi Su,Ming Dai,Mohammad Peydayesh,Zhou Dong,Qiyao Sun,Mattia Usuelli,Raffaele Mezzenga
Enzyme immobilization is an efficient and cost-effective approach to recovering, stabilizing, and enhancing enzyme catalytic properties. It is a challenge, however, for coimmobilized multiple enzymes to perform consecutive reactions without being inactivated under similar conditions. Here, we present a facile enzyme immobilization platform using β-lactoglobulin amyloid fibril hydrogels. Two different hydrogels, loading either RuBisCO alone (hereby termed AFR*) or seven enzymes related to the Calvin Cycle (hereby termed AF7E hydrogel), show immobilization efficiency of over ∼95% while simultaneously exhibiting excellent activity and stability. The AFR* hydrogel enables the fixation of CO2 into 3-phosphoglycerate (3-PGA), which is then utilized as the initial step in the Calvin Cycle cascade catalytic reactions if the AF7E hydrogel is used, mimicking the light-independent part of the more complex natural photosynthesis full process. The converted substrates of this process contain precursors (α-glycerophosphate dehydrogenase and dihydroxyacetone phosphate), which can be further converted to fructose by additional aldolase. Due to the proteinaceous nature of the amyloid substrate, the AF7E hydrogel is completely biodegradable by pepsin, as confirmed via atomic force microscopy and circular dichroism spectroscopy analysis. This original enzyme-amyloid hybrid is biocompatible, sustainable, and scalable and may serve as a general template for multienzymatic catalytic platforms.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Aicheng Song,Zhitao Han,Xiao Yang,Mengjing Zhang,Xi Wu,Zelu Zhou,Dong Liu,Dong Ma
The high energy consumption associated with solution regeneration in amine-based CO 2 capture processes remains a major challenge for large-scale carbon capture and storage (CCS) applications. However, the addition of solid acid catalyst accelerates the slow CO 2 desorption process while reducing the energy consumption for regeneration of the amine-rich solution. Herein, we innovatively developed Mn 3 O 4 -modified SAPO-34 catalysts via impregnation, demonstrating exceptional efficacy in reducing energy consumption for CO 2 -rich monoethanolamine (MEA) solution regeneration. Mn 15 -SAPO catalyst exhibited excellent performance in catalytic desorption tests using a 5 M CO 2 -rich MEA solution at 90 °C, achieving a 31.0 % increase in CO 2 desorption rate, a 133.3 % increase in CO 2 desorption amount, and a 57.1 % reduction in solution regeneration heat duty compared to the non-catalytic process. Comprehensive characterization revealed that the optimized Mn 15 -SAPO catalyst featured abundant strong acidic sites, optimal mesoporous structure, and the redox activity of Mn 3+ /Mn 4+ species. FTIR and 13 C NMR analysis confirmed the catalytic accelerating effect of catalysts on the conversion of intermediates. A possible reaction mechanism for the catalytic desorption of CO 2 over Mn x -SAPO catalysts was discussed. Additionally, the cycling stability of Mn 15 -SAPO catalyst was also evaluated. This work demonstrated the potential of Mn 15 -SAPO catalyst in enhancing the efficiency of the amine CO 2 capture process and reducing energy consumption, which was conducive to the application of industrial CO 2 capture.
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REACTIVE & FUNCTIONAL POLYMERS
·
2025
·
IF 5.1
Waseem Tariq,Manoj Pudukudy,Li Shuangjiang,Yi Liu,Heping Su,Xiliang Li,Yunfei Zhi,Shaoyun Shan
The soaring levels of atmospheric carbon dioxide (CO 2 ), driven by fossil fuel consumption, pose significant environmental challenges, necessitating innovative strategies for its mitigation and utilization. This study introduces a novel, metal-free nitrogen-rich organic polymer, CMBr-OP, designed as an efficient catalyst for the cycloaddition of CO 2 with epoxides to produce cyclic carbonates. Synthesized through a straightforward one-step polymerization of cyanuric chloride and melamine, followed by functionalization with bromoacetic acid, CMBr-OP integrates multiple active sites, including nitrogen-rich triazine units and bromine functionalities, which synergistically enhance catalytic performance. Under mild reaction conditions (110 °C, 1 MPa CO 2 pressure, 6 h), CMBr-OP achieves an impressive 99.6 % yield of chloropropene carbonate without requiring co-catalysts or solvents. Comprehensive characterization techniques, including FTIR, XPS, SEM, and BET analysis, confirm its hierarchical porous structure, high surface area, and uniform distribution of active sites, facilitating efficient CO 2 activation and epoxide ring-opening. The catalyst demonstrates remarkable versatility, effectively catalyzing a wide range of epoxides, and exhibits excellent recyclability, maintaining high activity over five consecutive reaction cycles. DFT calculations reveal the critical role of hydrogen bond donors, nitrogen sites, and bromide ions in activating both epoxides and CO 2 , underscoring the cooperative synergy within CMBr-OP. This work represents a significant advancement in sustainable catalytic systems for CO 2 utilization, aligning with green chemistry principles and offering a promising candidate for industrial-scale applications aimed at reducing CO 2 emissions and promoting environmentally friendly chemical processes.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Wangjiang Gao,Chenglong Wang,Hexing Yang,Chunjing Ran,Shengzhou Xu,Dan Ren
Optimizing the electrocatalytic interface for the electroreduction of carbon dioxide (CO 2 ) in acid through the usage of cations in the electrolyte has shown its effectiveness in enhancing CO 2 conversion efficiency. However, such a positive impact in promoting CO 2 activation is limited by the solubility of salt, hence alternative ways to optimize the interface shall be sought for. Here, the hydrophobicity of the catalytic interface is tuned through the judicious design of a sandwich-like structure by covering the catalytic copper layer with polytetrafluoroethylene (PTFE) particles. After optimizing the thickness of the PTFE layer on a commercial CuO X nanoparticle catalyst, an improved FE for multi-carbon products from 35.0% to 59.3% in 0.05 m H 2 SO 4 electrolyte with the addition of 0.8 m K + (pH = 1.6) is achieved. Moreover, in situ Raman spectroscopy proves that the hydrophobic layer facilitates the formation of * CO intermediates and promotes the transition of bridge-bonded * CO to atop-bonded * CO. The reduction of carbon monoxide (CO) is further performed at different partial pressures to reveal the critical role of * CO coverage for the formation of multi-carbon products. Collectively, it is proposed that the optimized hydrophobic modification of the catalyst effectively tunes the coverage of * CO intermediate as well as reduces the available water molecules at the interface, thereby promoting the formation of multi-carbon products and simultaneously suppressing hydrogen evolution reaction. The study illustrates a new venue toward improving the efficiency of CO 2 conversion in acid.
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FUEL PROCESSING TECHNOLOGY
·
2025
·
IF 7.7
Jinxu Hao,Xianda Sun,Baibin Ma,Wanzhen Huang,Yuandong Yang,Xiaohan Ren
The carbon-neutral and carbon-negative energy utilization technologies have long been people pursued to realize the strategic objective of carbon neutrality. Herein, we propose a cation-exchange membrane (CEM) direct formate-CO 2 fuel cell that possesses the capability of simultaneously generating electricity and producing hydrogen, as well as continuously transforming carbon dioxide into pure sodium bicarbonate. Using the CO 2 -derived formate fuel, the roof-of-concept CEM direct formate-CO 2 fuel cell exhibits a peak power density of 38 mW cm −2 at 80 °C without the assistance of additional electrolyte. The fairly stable constant-current discharge curve along with the detected hydrogen and pure sodium bicarbonate prove the conceptual feasibility of this electricity‑hydrogen-bicarbonate co-production device. By adding alkaline electrolyte to the anode, we achieved a higher peak power density of 63 mW cm −2 at the corresponding hydrogen production rate of 0.57 mL min −1 cm −2 . More interestingly, the concentrations of pure NaHCO 3 solution can be controlled by adjusting the cathode water flow rate and fuel cell discharge current density. This work presents a theoretically feasible avenue for coupling hydrogen production and CO 2 utilization.
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