JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2022
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IF 10.319
Yidu Wang,Jingnan Ding,Jun Zhao,Jiajun Wang,Xiaopeng Han,Yida Deng,Wenbin Hu
Constructing nanohybrids with a synergistic effect using multi-components and specific micro/nanostructures can significantly enhance their electrocatalytic activity. In this work, we fabricated an In 2 O 3 ⊃NC@GO nanohybrid, in which In 2 O 3 nanoparticles (NPs) were encapsulated by an N-doped carbon (NC) shell and supported on graphene. The multi-components in In 2 O 3 ⊃NC@GO synergistically optimize the structural and electronic properties of the material. The particle size and dispersion of In 2 O 3 NPs were optimized owing to the separation effect of the amorphous NC shell and graphene support. This separation effect exposes more number of active sites for the electrochemical reaction. Abundant oxygen vacancies exist in In 2 O 3 , leading to a stronger ability for the adsorption and activation of CO 2 . The NC shell inhibits the direct contact between the electrolyte and In 2 O 3 , which significantly suppresses competitive H 2 evolution. The charge transfer during the electrocatalysis process is also effectively enhanced due to the carbon components. The synergistic effect of multi-components in the In 2 O 3 ⊃NC@GO sample results in a significantly improved CO 2 reduction reaction performance with a high HCOO – Faradic efficiency (FE) of 91.2% and a current density of 40.38 mA cm –2 at –0.8 V obtained using a flow cell. The present work demonstrates that rationally designing nanohybrids with multifunctional components is an effective strategy for optimizing the structural and electrocatalytic properties of materials for energy conversion.
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Journal of Materials Chemistry A
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2022
·Vol. 10
·期 10
·5540-5549
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IF 14.511
Zixuan Xu,Ke Liu,He Huang,Yadong Zhang,Zhouyang Long,Minman Tong,Guojian Chen
In this work, we reported a facile catalyst-free and initiator-free strategy to fabricate a new class of viologen-linked ionic polyacetylenes (denoted as VIPAs) that can achieve simultaneous ionization and polymerization in one-pot and one-step. To our surprise, the ionic polymers VIPA-X (X = Br or Cl) were directly synthesized by quaternization-induced in situ polymerization from commercially available 4,4′-bipyridine with propargyl bromide or propargyl chloride. It was found that reaction temperatures have a remarkable influence on the synthesis of VIPAs, achieving the transformation from soluble oligomers to insoluble highly cross-linked polymers by adjusting the temperatures from 30 °C to 100 °C. At a higher temperature of 100 °C, the obtained highly cross-linked ionic polymers VIPA-Br and VIPA-Cl were insoluble in both hot water and even dimethyl sulfoxide (DMSO). By virtue of abundant halogen anions and the absorbed H-bonded water, both VIPA-Br and VIPA-Cl were employed as efficient heterogeneous catalysts for the conversion of CO2 with various epoxides into cyclic carbonates at atmospheric pressure and low temperatures. In particular, the catalytic activities of VIPA-Br for the conversion of various epoxides are much better than those of VIPA-Cl at low temperatures, which should be attributed to the higher nucleophilicity and better leaving ability of the Br− anion than those of the Cl− anion. The present work affords a succinct catalyst-free strategy to construct more task-specific ionic polyacetylenes by quaternization-induced polymerization of multi-N-heterocycle monomers and propargyl halides towards diverse applications.
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ULTRASONICS SONOCHEMISTRY
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2022
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IF 9.336
Hanyang Gao,Kunkun Pei,Guoxin Hu,Wenxing Liu,Aihua Meng,Hongcheng Wang,Huifeng Shao,Wenxin Li
CO 2 -expanded organic solvent is a kind of important fluid medium and has broad applications in chemical industry, environmental protection and other fields. Ultrasonic cavitation in gas expanded liquids (GXLs) is conducive to enhancing mass transfer and producing many exciting phenomena. In this paper, the ultrasonic cavitations and streaming in the saturated CO 2 -expanded liquid N, N-dimethylformamide (DMF) at 4.2 MPa and 5.2 MPa are observed by a high-speed camera. The cavitation intensity and time trace of pressure pulses are recorded using a PZT hydrophone. The influences of gas–liquid equilibrium pressure and ultrasonic power on the cluster dynamics of transient and stable cavitation are examined. The excess molar enthalpies required for CO 2 dissociation from DMF are calculated by Peng-Robinson equations of state and the change of surface free energy of CO 2 -expanded DMF is predicted. The results show that the excess enthalpy of the mixture is one of the key factors to control ultrasonic cavitation at high pressurized conditions, while the surface tension is the key factor for low pressure. As the increase of applied ultrasonic power, the formation and collapsing frequency of bubble clusters increases, and the amplitude and cyclic frequency of pressure pulse are enhanced. The transient cavitation intensity increases as it reaches a maximum value at a certain ultrasonic power and then decreases. The change trends of stable cavitation intensity under different pressures are basically same. It can be concluded from the evidence that ultrasonic cavitation in CO 2 -expanded DMF is affected by the combined effect of compression and substitution: compression depresses the nucleation and growth of bubbles, while the high solubility of CO 2 in DMF is conducive to the generation of bubbles in cavitation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Xiaoyu Li,Ruihong Li,Kang Peng,Liangjie Fu,Keping Zhao,Haoran Li,Jiahui Peng,Luxue Wang
Cyclic CO 2 adsorption via solid amine adsorbents is widely considered as a feasible technology for CO 2 mitigation from industrial flue gas. However, the high cost and rapid decline of adsorption capacity and insufficient cyclic stability limit their large-scale application. Herein, we demonstrated a facile and efficient interlayer functionalization approach, involving the synthesis of acid activated expanded vermiculite derived silica (AEV) support with hierarchical layered porous structure and the impregnation of PEI into the AEV support, to enhance CO 2 adsorption capacity and cycle stability of AEV/PEI adsorbents. The optimal AEVP50 adsorbent exhibited a high CO 2 uptake of 2.21 mmol/g at 75 °C and stable cyclic stability with a mere 1% decay after 10 cycles, owing to the superior hierarchical porous structure of synthesized AEV support. The interlayer functionalization of vermiculite was beneficial for enlarging interlayer volume and producing hierarchical porous structure and abundant Lewis acid sites, which could increase PEI loading content, form uniform amine distribution with less blocked pores/channels and enhance the interfacial interaction between PEI and AEV support. Furthermore, the interlayer spatial confinement effect significantly avoids the inactivation of functional amidogen during the regeneration stage. This strategy significantly enhanced the cyclic CO 2 adsorption of AEV/PEI adsorbents through the interlayer functionalization of VMT, and is promising for various practical CO 2 capture and separation processes.
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Journal of Physical Chemistry C
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2022
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IF 4.177
Yuyao Zhang,Yu Tian,Wen Chen,Min Zhou,Siyong Ou,Yueli Liu
The CO2 photoreduction process is becoming a promising strategy to solve the energy shortage problem and global warming in recent years. How to promote the separation of photoinduced carriers has attracted attention for the improvement of photocatalytic CO2 reduction. In the present work, an S-scheme heterojunction of Bismuthene/CsPbBr3 quantum dots (Bismuthene/CsPbBr3 QDs) is constructed as the photocatalyst for CO2 conversion. As a result, Bismuthene/CsPbBr3 QDs exhibit an optimal CH4 evolution rate of 43.1 μmol h–1 g–1 with 84.53% selectivity over CH4 under ultraviolet–vis light (UV–vis) irradiation. Construction of the S-scheme heterojunction with a narrow band gap semiconductor is the main factor for improving the photocatalytic performance, as the S-scheme heterojunction can suppress the recombination of photoinduced carriers and retain redox ability. The narrow band gap semiconductor Bismuthene can enhance light absorption abilities. This work probably provides some insights for the designing of heterojunction photocatalysts and the improvement of photocatalytic performance.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Boyu Li,Jiaxiang Liu,Xuanting He,Rong Wang,Wenquan Tao,Zhuo Li
Facilitated transport mixed matrix membranes (FTMMMs) separation technology has shown advantages in improving CO 2 recycling efficiency and reducing the environmental impacts associated with carbon emission. The design of FTMMMs is highly dependent on the selection of a compatible combination of polymer and filler. Herein, a novel grafted nanoparticles (GNPs) filler UiO-66-NM@PEG with multiple groups prone to hydrogen bond was designed to alleviate the phase separation and performance degradation caused by filler/polymer poor compatibility. In the GNPs configuration, by employing the coexistence strategy of coupling reaction and covalent bonds , maleic anhydride (MAH) was coupled with the amino group on UiO-66-NH 2 without clogging or cracking, and the generated carboxyl groups can be cross-linked with the hydroxyl groups on the poly (ethylene glycol) (PEG) by covalent bonds. The UiO-66-NM@PEG demonstrated excellent interface compatibility between the filler and matrix phase of UiO-66-NM@PEG/PVDF, which was further convinced by molecular modelling. The resultant UiO-66-NM@PEG/PVDF achieved a simultaneous enhancement of gas permeability (537.6 Barrer) and ideal CO 2 /N 2 selectivity (47.8), which surpassed Robenson upper bound. Moreover, the UiO-66-NM@PEG/PVDF has a lasting sustainability over 960 h (40 days), and a valid anti-acid/alkali corrosion resistance in harsh environments. More importantly, UiO-66-NM@PEG can also be well mixed with other mixture matrices such as hydroxy-terminated polydimethylsiloxane (PDMS) and polyether-block-polyamide copolymer (PEBAX) to promote permeability/ideal selectivity up to (724.1 Barrer/21.1) and (307.4 Barrer/31.4). We thus concluded that this rational-design GNPs approach provides a general toolbox for controllable engineering in GNPs whereby enhanced favorable filler/matrix compatibility in FTMMMs with optimized CO 2 /N 2 separation properties.
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ACS Omega
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2023
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IF 4.1
Xintong Wang,Jiang Yang,Xu Chen,Kunfeng Yan
Two food flavors, furfuryl mercaptan (2-FFT) and difurfuryl disulfide (DFDS), were investigated as green corrosion inhibitors for the N80 steel in a CO2-saturated solution containing 3.5% NaCl. Experimental methods, quantum chemical calculations, and molecular dynamics simulation were employed to evaluate the effectiveness of 2-FFT and DFDS. The results of the study indicate that both 2-FFT and DFDS act as mixed corrosion inhibitors, with a dominant inhibition effect on the cathodic reaction. 2-FFT is physiochemically adsorbed on the steel surface in a tiled form through the furan ring and the – SH groups as adsorption sites. On the other hand, DFDS is chemisorbed on the steel surface through the – S–S– groups in a parallel manner. DFDS exhibits a higher tendency for electron transfer and stronger adsorption to steel compared to 2-FFT. Overall, this study highlights the potential of natural food flavors as effective and environmentally friendly corrosion inhibitors for carbon steel in CO2-saturated environments. The findings of this research can contribute to the development of sustainable and nontoxic corrosion inhibitors for the oil and gas industry.
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Journal of CO2 Utilization
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2023
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IF 7.7
Zhongzheng Zhang,Lina Zhang,Qiang Gao,Nannan Sun,Wei Wei
Nitrogen (N)-doped microporous hollow carbon spheres were prepared by facilely nanocasting spherical SiO 2 with N-containing melamine phenolic resin through a simple in-situ polymerization process. Through regulating the dosage of melamine, N content in microporous hollow carbons could be easily tuned to an unprecedented level of 49.2 wt%. Additionally, in order to address the common problem of relatively poor structural porosity of N-doped carbons, especially after incorporating vast N into carbon frameworks in reported literature, a comprehensive strategy including optimizing carbonization temperature and performing further activation by CO 2 and KOH were explored, and their effects on material textural properties and CO 2 capacity were systematically studied. Although this strategy did not completely avoid the N loss during activation of carbon materials, it sharply promoted the textural properties of carbon materials at the expenses of partial N and efficiently produced a series of highly microporous carbon materials, still with abundant N species (11.5 ∼ 29.9 wt%) and large structural porosity (330 ∼ 1263 m 2 /g). More importantly, these N-doped microporous hollow carbons, when used for CO 2 capture, showed superior CO 2 capacities of 3.00 mmol/g (25 °C and 1 bar) and 1.05 mmol/g (40 °C and 0.1 bar), exceptionally robust cyclic stability, and low regeneration energy of 2.75 GJ/ton CO 2 , which is much lower than aqueous amine-based absorbents and comparable to amine-supported adsorbents. Thus, these outstanding adsorption performances make the N-doped microporous hollow carbon spheres prepared in this study more promising for energy-effective CO 2 capture from dilute gas streams.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Xiaoyang Chen,Jian Chen,Yijie Liu,Yang Liu,Yun Gao,Siwei Fan,Xiangxi He,Xiaohao Liu,Chao Shen,Yong Jiang,Li Li,Yun Qiao,Shulei Chou
Metal–CO2 batteries, especially Li–CO2 and Na–CO2 batteries, are regarded as ideal new-generation energy storage systems owing to their high energy density and extraordinary CO2 capture capability. However, the advancement of metal–CO2 batteries is still at an early stage. The problems caused by accumulation of carbonates during charge–discharge cycles, such as large polarization and poor reversibility, restrict their practical application. Therefore, designing efficient catalysts is crucial for promoting the decomposition of carbonate to improve the electrochemical performance of metal–CO2 batteries. Herein, we first adopted sea urchin-like γ-MnO2 as the cathode material for Li/Na–CO2 batteries. Benefiting from the unique structure and excellent catalytic activity of γ-MnO2, the as-prepared Li–CO2 and Na–CO2 batteries can achieve low overpotentials of 1.28 and 1.36 V, respectively, at a current density of 100 mA g–1 with a cutoff capacity of 1000 mA h g–1. The overpotentials are lower than those of most of the state-of-the-art catalysts in previous reports. After 100 and 50 cycles of Li–CO2 and Na–CO2 batteries, respectively, their charging termination voltages remain at around 4.1 and 3.9 V, respectively; such a low charging platform indicates the excellent catalytic activity of the γ-MnO2 cathode on the discharge products. Our findings offer a promising guideline to design efficient electrocatalysts for high-performance metal–CO2 batteries.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jiaying Yan,Yayu Guan,Barbara Marchetti,Yuyu Liu,Fanghua Ning,Jin Yi,Xiao-Dong Zhou
Electrochemical reduction of CO 2 (ERCO 2 ) is an effective way to convert CO 2 into useful chemical products. However, most catalysts used for ERCO 2 show poor selectivity and stability. Here, we design a Bi 8 Eu 1 bimetallic catalyst, which exhibits both excellent stability (>400 h) and Faradaic efficiency for formate production (∼100% at − 0.89 V RHE ). Moreover, high Faradaic efficiency (>97%) is observed over a wide potential window (from − 0.89 V RHE to − 1.19 V RHE ). In a flow-cell, the Bi 8 Eu 1 catalyst shows an ultra-high current density of 250 mA cm −2 at − 0.77 V RHE . Density functional theory calculations indicate that the Bi-Eu interactions activate the Bi sites for strongly stabilizing *OCHO intermediates, thus promoting the conversion of CO 2 to formate. This work provides insights into the design of excellent electrocatalysts for ERCO 2 with improved activity and durability.
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Journal of Energy Chemistry
·
2023
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IF 13.1
Hua-Qing Yin,Zuo-Shu Sun,Qiu-Ping Zhao,Lu-Lu Yang,Tong-Bu Lu,Zhi-Ming Zhang
Traditional urea synthesis under harsh conditions is usually associated with high energy input and has aroused severe environmental concerns. Electrocatalytic C–N coupling by converting nitrate and CO 2 into urea under ambient conditions represents a promising alternative process. But it was still limited by the strong competition between nitrate electrochemical reduction (NO 3 ER) and CO 2 electrochemical reduction (CO 2 ER). Here, Fe II -Fe III OOH@BiVO 4 - n heterostructures are constructed through hydrothermal synthesis and exhibited superior performance toward urea electrosynthesis with NO 3 − and CO 2 as feedstocks. The optimized urea yield and Faradaic efficiency over Fe II -Fe III OOH@BiVO 4 -2 can reach 13.8 mmol h −1 g −1 and 11.5% at −0.8 V vs. reversible hydrogen electrode, which is much higher than that of bare FeOOH (3.2 mmol h −1 g −1 and 1.3%), pristine BiVO 4 (2.0 mmol h −1 g −1 and 5.4%), and the other Fe II -Fe III OOH@BiVO 4 - n ( n = 1, 3, 5) heterostructures. Systematic experiments have verified that BiVO 4 and FeOOH are subreaction active sites towards simultaneous CO 2 ER and NO 3 ER, respectively, achieving co-activation of CO 2 and NO 3 − on Fe II -Fe III OOH@BiVO 4 -2. Moreover, the urea synthesis via the *CO and NO* intermediates and C–N coupling was confirmed by the in situ Fourier transform infrared spectroscopy. This work not only alleviates the CO 2 emission and nitrate pollution but also presents an efficient catalyst for synergistic catalysis towards sustainable urea synthesis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Shujie Liang,Xiaohui Zhong,Zuqi Zhong,Hong Deng,Wai-Yeung Wong
Photoconversion of CO 2 into value-added fuels has aroused widespread interest; however, this process is significantly limited by the inefficient thermodynamics and sluggish reaction dynamics in the diluted CO 2 . To circumvent these obstacles, we design a bipyridine-based polyimide polymer for anchoring single Ni site for diluted CO 2 photoreduction. The desired Ni single atomic catalysts achieve high generation activity of ∼ 2262 μmol/h with apparent quantum efficiency (A.Q.E.) of 0.20% for CO 2 -to-CO in 0.1 atm CO 2 pressure. No measurable H 2 is produced in the catalytic process, affording nearly 100% CO selectivity over water splitting. This superior activity and selectivity outperform most previous atomical catalysts. Mechanistic analyses elucidate that the highly dispersed Ni atoms act as active sites for effective CO 2 binding and activation, and stabilize the rate-determining step of intermediates for CO generation. This work discloses the relationship between catalytic properties and single atoms for efficient solar-driven diluted CO 2 reduction.
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