ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Hongbo Xue,Congcong Yin,Sen Xiong,Jingying Yang,Yong Wang
Solar energy-driven reduction of CO2 into fuels with H2O as a sacrificial agent is a challenging but desirable subject in photosynthesis. Covalent organic frameworks (COFs) are considered promising candidates for this subject because of their designable structures and functions. The coordination of transition metal ions into COFs is a feasible way to boost the photocatalytic activity. However, postsynthetic modification of COFs with metal ions often leads to a significant decrease in crystallinity and the specific surface area. Herein, we develop a one-pot synthesis of metal-coordinated (nonnoble metal) COFs with high crystallinity. HB-TAPT + Co with ordered and segregated D–A arrays is synthesized by combining 2,4,6-tris(4-aminophenyl)-1,3,5-triazine (TAPT, a strong electron-acceptor) with 2-hydroxy-1,3,5-benzenetricarbaldehyde (HB)-loaded Co2+ (a strong electron-donor). The CO production when using HB-TAPT + Co under visible light irradiation for 4 h is 78.4 μmol g–1, which is 3.2 times that of HB-TAPT + Co synthesized by the postsynthetic modification method and 2.65 times that of HB-TAPT without the metal ions. HB-TAPT + Co also has good recycling stability in photocatalytic CO2 reduction. Additionally, experimental results have demonstrated that the crystallinities of these metal-coordinated materials contribute greatly to the conversion of CO2 in the photoreaction with H2O. This work provides a new protocol for improving the CO2 photoreduction performance by coordinating metal ions to COFs while maintaining the original crystallinity through a one-pot synthesis method.
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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Tianfen Huang,Ruiyi Wang,Jin Zhang,Jiapei Wang,Hui Ge,Jun Ren,Zhanfeng Zheng
Graphitic carbon nitride (g-C 3 N 4 ) based materials has been widely used for catalytic CO 2 hydrogenation reaction. However, the catalytic activity is restricted due to the barren active sites and the weak ability to activate CO 2 for the traditional g-C 3 N 4 . We demonstrate here that cyano group modified g-C 3 N 4 supported Ru nanoparticles exhibits high activity and selectivity for CO 2 methanation. The introduction of cyano group promotes the formation of medium basic sites for enhanced CO 2 adsorption. Meanwhile, the formation of electron-rich Ru nanoparticles with the assistance of cyano group boosts the H 2 activation. The synergistic effect of cyano group and Ru nanoparticles improves catalytic performance up to 14 times. Characterizations prove that cyano group with electron-withdrawing properties influences the way of CO 2 adsorption via electron transfer and changes the CO 2 hydrogenation reaction pathway. This work provides a new insight into the switching of CO 2 hydrogenation pathway and enhanced catalytic activity via surface functional groups modification of g-C 3 N 4 based catalyst.
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INORGANIC CHEMISTRY
·
2023
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IF 4.6
Didi Dong,Xinyu Zhao,Chun Pu,Yao Yao,Bo Zhao,Ge Tian,Ganggang Chang,Xiaoyu Yang
Hybridization of metal–organic frameworks (MOFs) and homogeneous ionic liquids (ILs) endows the heterogeneous composite with high porosity and accessible multiple active sites (e.g., acidic or basic sites), which exhibits great potential in CO2 capture and conversion. Nevertheless, the majority of MOF composites are synthesized as powders, significantly restricting their practical applications due to inherent problems such as poor handling properties, high pressure drops, and mechanical instability. Thus, it is crucial to shape MOF composites into various monoliths that allow efficient processing, especially for industrial purposes. In this work, a hierarchical ILs@nanoMOF composite gel (H-IL@UiO-66-gel) featuring both intraparticle micropores and interparticle mesopores and multiple active sites was successfully fabricated by a two-step approach. Benefiting from the integrated advantages of the hierarchically porous MOF for enhanced mass transfer and affinity of ILs for activating CO2 molecules, the resultant H-IL@UiO-66-gel exhibits excellent uptake of macromolecules and catalytic activity toward CO2 cycloaddition with epoxides under moderate conditions, far beyond the traditional microporous IL@UiO-66-gel and unfunctionalized H-UiO-66-gel. Furthermore, the H-IL@UiO-66 composite monolith can be effortlessly separated and reused at least three times without depletion of catalytic activity. It is believed that this fabrication method for the shaping of MOF composites is highly versatile and can be extended to other types of MOFs for various application fields.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hao Guo,Likun Luan,Jinde Cai,Xiuling Ji,Haijun Yu,Yuhong Huang
CO 2 activation and conversion by enzymes to produce value-added multi-carbon compounds under mild conditions show significant impact on carbon neutrality. However, the enzyme co-factor NADH is expensive and the regeneration is still challenging for the enzyme reaction process. Inspired by natural photosynthesis, this study successfully developed a biomimetic photocatalyst Ce/TCPP-UiO-66-NH 2 (TCPP: meso-tetrakis (4-carboxyphenyl) porphine) for NADH regeneration and CO 2 activation. Structure analysis and spectra showed that the co-doping of Ce and TCPP reduced the band gap width of UiO-66-NH 2 , improved the separation efficiency of photo-generated carriers, and endowed it with excellent photocatalytic performance. The synthesized biomimetic photocatalyst Ce/TCPP-UiO-66-NH 2 was then applied for NADH regeneration. The regeneration efficiency of NADH can reach up to 95 % after 3 h of light reaction, which was about 1.6 times higher than that of the control group. Ultra-fast femtosecond time-resolved transient absorption (fs-TA) showed that Ce/TCPP-UiO-66-NH 2 possessed the shortest average decay time ( τ ¯ = 1.12 ps), indicating shorter average life-time of carriers after Ce doping, thus suppressing hole-electron recombination. Finally, the key enzyme formate dehydrogenase (FDHPa) for CO 2 activation was immobilized on the membrane, combining with light regeneration of NADH for CO 2 production to formate. The formate yield (3.1 mM) was 16 times higher than that of the control group (0.19 mM). This work provided an effective strategy and efficient photocatalyst for the biomimetic photocatalytic activation of CO 2 to formate, which is an indispensable bridge for the further high-valuable C n compounds production by biocatalysis.
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POLYMER
·
2023
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IF 4.6
Haiming Liu,Xiangdong Wang,Hao-Yang Mi,Maxwell Fordjour Antwi-Afari,Chuntai Liu
Polyimide foams (PIFs) are usually synthesized by solution polymerization , followed by chemical foaming to prepare thermosetting foam. In this research, lightweight microcellular thermoplastic polyimide foams (TPIFs) were fabricated via a novel two-step foaming approach using supercritical carbon dioxide (scCO 2 ) as a blowing agent. The poly(amic acid) (PAA) and polyester ammonium salt (PEAS) precursor solutions were synthesized with pyromellitic dianhydride (PMDA) as dianhydride reagents and polyether amine Jeffamine D230 as aliphatic diamine reagent via blending and solution polymerization, respectively. The solution polymerization process demonstrated a higher molecular weight and superior formability than the blending process. The optimum thermal imidization temperature of 200 °C was optimized via the thermal and rheological property analysis. The cell morphology and mechanical properties of the TPIFs could be turned by varying the saturation time, foaming pressure, and imidization temperature. At a thermal imidization temperature of 200 °C, the TPIFs exhibited a branched structure with a small mean cell diameter (123.78 μm), and a high compressive strength (0.4 MPa) under 10 % strain at high temperature and pressure, which was more than ten times that of the TPIFs with thermal imidization temperature of 130 °C. This research provides a feasible method for producing high volume expansion ratio TPIFs with adjustable microcellular structures and outstanding mechanical properties.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
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IF 19.503
Shao-Hai Li,Ming-Yu Qi,Yun-Yan Fan,Ye Yang,Masakazu Anpo,Yoichi M.A. Yamada,Zi-Rong Tang,Yi-Jun Xu
Molecular transition metal complexes are widely explored in artificial photosynthetic redox catalysis due to their extraordinary properties. However, these catalysts generally suffer from the intrinsic thresholds of photon harvesting efficiency and spectrum response range, greatly limiting their further applications. Polypyridyl ruthenium ( Ru ) has been perceived as a paradigmatic photosensitizer in CO 2 reduction systems but seldomly maneuvered. Herein, we develop a novel and practicable pseudo-supramolecular assembly at a molecular scale by conjugation with ultra-small nitrogen-doped carbon quantum dots (NCQDs) as ultraviolet-visible (UV–vis) light chromophore for enhanced photochemical conversion of CO 2 to CO. The reversible self-assembly of NCQDs with Ru is driven by dynamic non-covalent π-conjugated and electrostatic interactions. Femtosecond transient absorption and time-resolved fluorescence decay spectra combined with control experiment results collaboratively demonstrate that vectorial photo-induced exciton cascade occurs by means of their unique photophysical properties in the as-assembled NCQDs/ Ru dyad, enabling the superior photosensitized CO 2 reduction performance in both homogeneous and heterogeneous systems. This work is expected to not only shed new light on the development of promising artificial light-harvesting systems but also promote the implementation of metal complex-based systems for photoredox-catalyzed reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Zhikun Liu,Tao Yan,Han Shi,Hui Pan,Peng Kang
Direct electrochemical CO 2 capture and utilization from flue gas offers appealing route to closing the carbon cycle and avoiding the cost for CO 2 purification. Yet, the low CO 2 concentration in flue gas and competing oxygen reduction reaction (ORR) pose severe challenges for this process. Herein, we report 4-aminobutylphosphonic acid ligand layer capped Ag nanoparticles (NH 2 BPA-Ag) for high-efficiency conversion of simulated flue gas (SFG). The amino group in NH 2 BPA is available for CO 2 capture and activation, while phosphonic acid groups inhibit ORR by desorbing *OOH intermediate. NH 2 BPA-Ag achieves 82% CO Faradaic efficiency (FE CO ) in H-cell for SFG reduction and enhances FE CO 2.6 times over pristine Ag nanoparticles. In a membrane electrode assembly electrolyzer, NH 2 BPA-Ag shows 79.6% FE CO and 38.1% full-cell energy efficiency at 48 mA cm -2 for SFG conversion. This study highlights the strategy of tailoring catalytic microenvironments at molecular level for realizing a highly selective performance.
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FUEL
·
2023
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IF 7.4
Huan Wang,Xueyin Zhang,Zhipeng Su,Tiehong Chen
Oxidative dehydrogenation of propane in the presence of carbon dioxide (CO 2 ) effectively promotes the utilization of alkanes and CO 2 to produce high value-added olefins and carbon monoxide products. In this work, bimetallic PtCo nanoparticles with diameter of 1–2.5 nm loaded on dealuminated nano-Beta zeolite were successfully prepared for propane oxidative dehydrogenation with CO 2 . The silanol groups formed after dealuminization of nano-Beta zeolite acted as the anchoring sites to enhance the dispersion of PtCo nanoparticles , and the introduction of Co further promoted the uniform distribution of Pt, resulting in smaller bimetallic PtCo nanoparticles. By optimizing the Pt/Co ratio, the conversion of propane and CO 2 at 550 °C was as high as 51.8 % and 30.6 %, respectively. The dealuminized Beta supported PtCo nanoparticles exhibited high stability during the reaction, and there was no obvious aggregation of PtCo nanoparticles after 6 h on stream. In this study, the highly efficient catalyst prepared by impregnation method using modified commercial zeolite as the carrier is suitable for large-scale production and shows great practical prospect in the application of propane oxidative dehydrogenation with CO 2 .
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LANGMUIR
·
2023
·
IF 3.9
Hanwen Wang,Hangyuan Zhang,Qian Wu,Boyi Zhang,Zehua Zhang,Xiaoping Rao
Designing stimulus-switch viscoelastic solutions and Pickering emulsions with reversible CO2-responsive behavior remains a challenge. A rosin-based CO2-responsive surfactant, N-cetyl-maleimidepimaric acid N,N-dimethylenediamide (C16MPAN), was synthesized and used to prepare CO2-triggered viscoelastic solutions and Pickering emulsions. This surfactant exhibited excellent CO2-responsive performance in water and formed a viscoelastic solution. This viscoelastic system was investigated by dynamic light scattering (DLS), rheology, and cryogenic transmission electron microscopy (Cory-TEM). The shear viscosity of the system increased by 3–4 orders of magnitude after bubbling with CO2 and a large number of elongated, flexible, tubular wormlike micelles were observed. Further, Pickering emulsions were prepared by C16MPAN+ synergistically with cellulose nanocrystals (CNCs), whose stability and switchability were investigated via adsorption isotherm, droplet size, contact angle, and macroscopic photographs. C16MPAN+ was adsorbed with CNCs to form mechanical barriers at the oil–water interface, making the emulsion stable for at least three months, and desorption from CNCs enabled emulsion breaking. The cycle could be switched reversibly multiple times and the particle size distribution of emulsion was basically the same. This work enriches the application of biomass resources in intelligent responsive materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chang Liu,Lingyu Shao,Chengjin Pan,Feng Xu,Zhicheng Wu,Zhongyang Zhao,Yaoji Chen,Haidong Fan,Chenghang Zheng,Xiang Gao
One of the major barriers in industrial applications of solvent-based CO 2 capture is the significant energy consumption required for absorbent regeneration. In this study, a novel multi-stage circulation (MSC) CO 2 absorption process was proposed, which implemented independent regulation of each stage, resulting in enhanced CO 2 capture performance and reduction of CO 2 regeneration duty. The MSC absorber was designed with four stages from bottom to top, each serving distinct functions, including CO 2 enrichment, CO 2 main absorption, CO 2 capture efficiency enhancement and aerosol capture. Simulation of the MSC process achieved a rich ethanolamine (MEA) solvent CO 2 loading of 0.512–0.570 mol CO 2 /mol amine, which was 8.1 %–9.9 % higher than typical process. The effects of test duration, amine solution flow rates, reaction temperatures and inlet CO 2 concentrations on CO 2 absorption performance were studied using the MSC experimental platform. The CO 2 regeneration duty reduced by over 13.2 % of the MSC process compared to a typical process using 25 wt% MEA solution and by over 22.9 % using piperazine (PZ)/N-methyldiethanolamine (MDEA) solution. Furthermore, the utilization of NH 3 /K 2 CO 3 solution achieved an energy consumption reduction of over 41.7 %, resulting in a CO 2 regeneration duty as low as 2.02 GJ/t CO 2 (1.84 GJ/t CO 2 , subtracting the heat loss). Meanwhile, potential strategies for optimizing parameters of MSC process were proposed to address the complex and volatile conditions.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 58
·122755-122773
·
IF 5.8
Guo Tianxiang,Wang Xilai,Xing Xiaodong,Fu Zhixiang,Ma Changxin,Bedane Alemayehu Hailu,Kong Lingfeng
This paper focuses on enhancing the performance of electrocatalytic CO 2 reduction reaction (CO 2 RR) by improving the dispersion of cobalt phthalocyanine (CoPc), especially for the methanol formation with multi-walled carbon nanotubes (CNTs) as a support. The promising CNTs-supported CoPc hybrid was prepared based on ball milling technique, and the surface morphology was characterized by means of those methods such as scanning electron microscopy (SEM), Fourier transform infrared spectrometer (FT-IR) and X-ray photoelectron spectra (XPS). Then, the synergistic effect of CNTs and ball milling on CO 2 RR performance was analyzed by those methods of cyclic voltammetry (CV), linear sweep voltammetry (LSV), electrochemical impedance spectroscopy (EIS), gas chromatography (GC), and proton nuclear magnetic resonance spectroscopy ( 1 HNMR). Subsequently, the reduction mechanism of CO 2 on ball-milled CoPc/CNTs was revealed based on the DFT calculations. The results showed that the electrocatalyst CoPc/CNTs hybrid prepared with sonication exhibited a conversion efficiency of CO 2 above 60% at -1.0 V vs. RHE, accompanied by the Faradaic efficiencies of nearly 50% for CO and 10% for methanol, respectively. The addition of CNTs as the support improved the utilization efficiency of CoPc and reduced the transfer resistance of species and electrons. Then the ball-milling method further improved the dispersion of CoPc on CNTs, which resulted in the fact that the methanol efficiency was raised by 6% and partial current density was increased by nearly 433%. The better dispersion of CoPc on CNTs adjusted the reduction pathway of CO 2 and resulted in the enhancement of methanol selectivity and catalytic activity of CO 2 . The probable pathway for methanol production was proposed as CO 2 → *CO 2 − → *COOH → *CO → *CHO → *CH 2 O → *OCH 3 → CH 3 OH. This suggests the significance of the ball-milling method during the preparation of better supported catalysts for CO 2 RR towards those high-valued products. Graphical Abstract
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ACS Omega
·
2023
·
IF 4.1
Shunyang Yao,Zhi Li,Zhen Liu,Xiaodong Geng,Li Dai,Yanmei Wang
Porosity is the key factor in determining the CO2 capture capacity for porous carbon-based adsorbents, especially narrow micropores of less than 1.0 nm. Unfortunately, this desired feature is still a great challenge to tailor micropores by an effective, low-corrosion, and environmentally friendly activating agent. Herein, we reported a suitable dynamic porogen of CuCl2 to engineer microporous carbons rich in narrow micropores of <1.0 nm for solving the above problem. The porosity can be easily tuned by varying the concentration of the CuCl2 porogen. The resultant porous carbons exhibited a multiscale micropore size, high micropore volume, and suitable surface nitrogen doping content, especially high-proportioned ultromicropores of <0.7 nm. As adsorbents for capturing CO2, the obtained microporous carbons possess satisfactory CO2 uptake, moderate heat of CO2 adsorption, reasonable CO2/N2 selectivity, and easy regeneration. Our work proposes an alternative way to design porous carbon-based adsorbents for efficiently capturing CO2 from the postcombustion flue gases. More importantly, this work opens up an almost-zero cost and industrially friendly route to convert biowaste into high-added-value adsorbents for CO2 capture in an industrial practical application.
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