ChemSusChem
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2018
·Vol. 11
·期 24
·4256-4261
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IF 7.411
Huajun Feng,Qiaoqi Guo,Yingfeng Xu,Ting Chen,Yuyang Zhou,Yigang Wang,Meizhen Wang,Dongsheng Shen
Photocatalytic conversion of CO 2 can provide a solution for simultaneously addressing global warming and solar fuel generation. However, its applicability is presently limited by the unsatisfactory photoconversion efficiency of the state-of-art photocatalysts. In this regard, enhancing CO 2 adsorption through surface modification could be an efficient way to improve the photoconversion efficiency. Herein, doping of nonpolar carbon quantum dots (CQDs) onto g-C 3 N 4 is reported for the construction of a metal-free heterojunction photocatalyst (CQDs/g-C 3 N 4 ). CQDs offer several advantages such as band-gap reduction and electron-withdrawing effect to improve light absorption and photocarrier separation efficiency. However, this study reveals that nonpolar CQDs could also improve CO 2 adsorption, photoinduced H 2 production, reaction kinetics, and alter CO 2 photoreduction pathways to generate CH 4 . Consequently, the CQDs/g-C 3 N 4 could generate six times more CO and CH 4 without detectable H 2 compared to pristine g-C 3 N 4 , under similar conditions. Therefore, this study demonstrates a promising strategy for efficient adsorption, activation, and subsequent photoreduction of CO 2 by nonpolar surface modification of g-C 3 N 4 . Graphical Fighting carbon with carbon : Incorporation of nonpolar carbon quantum dots on the surface of g-C 3 N 4 imparts several benefits, including band reduction, improved charge separation, and increased CO 2 adsorption. This enhances reaction kinetics and alters the pathways for photoreduction of CO 2 , thereby enabling efficient CO and CH 4 generation.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Kang An,Siran Zhang,Hong Wang,Ningyan Li,Ziyang Zhang,Yuan Liu
Direct hydrogenation of CO 2 into ethanol has been considered as an up-and-coming way to achieve CO 2 utilization. Ethanol can be generated by reverse water gas shift as well as CO hydrogenation over Co-based catalysts, where the regulation of Co 0 − Co δ+ is critical. Herein, we designed a supported Co-based catalyst doped with gallium, which was derived from Co-Al-O spinel precursor to facilitate synergistic catalyzing for CO 2 -to-ethanol transformation. The selectivity of ethanol reached 20.1 % in a continuous flow fixed micro-reactor over reduced CoGa 1.0 Al 1.0 O 4 /SiO 2 catalyst at 270 °C and 3.0 MPa. Results of characterization show that the existence of the strong interaction between Ga oxide and cobalt induced the configuration of Co 0 − Co δ+ active pairs, which promotes the process of ethanol synthesis by coupling the dissociation (CH x *)/non-dissociation (CO*) of the intermediates. The strategy by tuning the interaction between cobalt and gallium and/or aluminum oxide brings an avenue to tailor Co 0 − Co δ+ active pairs for the hydrogenation of CO and CO 2 .
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RSC Advances
·
2023
·Vol. 13
·期 23
·15998
·
IF 3.9
Jiehong He,Pin Lv,Jian Zhu,Hexing Li
Correction for ‘Selective CO 2 reduction to HCOOH on a Pt/In 2 O 3 /g-C 3 N 4 multifunctional visible-photocatalyst’ by Jiehong He et al. , RSC Adv. , 2020, 10 , 22460–22467, https://doi.org/10.1039/D0RA03959D .
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PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2010
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IF 3.203
Xingwei Yu,Zhi Wang,Zhihong Wei,Shuangjie Yuan,Juan Zhao,Jixiao Wang,Shichang Wang
A novel tertiary amine group containing fixed carrier thin film composite (TFC) membrane was developed by the interfacial polymerization of 3,3′-Diamino-N-methyldipropylamine (DNMDAm) and trimesoyl chloride (TMC) on the polysulfone (PS) support membrane. ATR-FTIR, XPS , AFM and SEM were employed to characterize the active surface of the composite membrane . The gas transport property of the DNMDAm-TMC/PS membrane was investigated by studying the permselectivity varying with feed gas pressure and the possible reactions between gases and the membrane. Furthermore, the effects of two important factors (the DNMDAm concentration and the TMC concentration) on membrane morphology and performance were investigated. It was found that both the DNMDAm concentration and the TMC concentration play important roles in determining the membrane morphology and performance, which may reconcile some contradictory findings in some references. Moreover, the DNMDAm-TMC/PS composite membrane showed both good CO 2 /N 2 and CO 2 /CH 4 separation performance. For CO 2 /N 2 gas mixture (20/80 by volume), the membrane prepared with 0.0062 mol/l of DNMDAm and 0.0226 mol/l of TMC displayed a CO 2 permeance of 173 GPU and CO 2 /N 2 selectivity of 70 at 0.11 MPa feed pressure. For CO 2 /CH 4 gas mixture (10/90 by volume), the same membrane showed a CO 2 permeance of 118 GPU and CO 2 /CH 4 selectivity of 37 at 0.11 MPa feed pressure. The high CO 2 /N 2 and CO 2 /CH 4 separation performance of DNMDAm-TMC/PS composite membrane was mainly attributed to the thin film thickness and the properties of tertiary amino groups.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2012
·
IF 1.693
Jiangfeng Yang,Qiang Zhao,Hong Xu,Libo Li,Jinxiang Dong,Jinping Li
We prepared several different surfaces and pore volumes on small pore zeolites by hydrothermal synthesis and ion exchange (Li+, Na+, and Ca2+) based on three basic gas diameter grade structures of zeolites: KFI (0.39 × 0.39 nm), CHA (0.38 × 0.38 nm), and LEV (0.36 × 0.48 nm), which were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and elemental analysis. The surface area and microporous volumes were calculated using the Dubinin–Radushkevitch (D-R) equation based on CO2 adsorption at 273 K. The CHA was synthesized with a lower Si/Al ratio, and the surfaces and microporous volumes were changed greatly by ion exchange. KFI had a higher Si/Al ratio, and the scope of the surface could be kept smaller. Focusing on the CO2, CH4, and N2 adsorption isotherms at high pressure (1 MPa), we found that the samples were exchanged by Li+ and Na+ with bigger surfaces and greater adsorption volumes. The orifice diameter was very important in the sieving of CO2 and N2 or CO2 and CH4, while Na-LEV had an excellent sieving effect because N2 and CH4 could not diffuse into its structure like CO2. From the viewpoint of the separate adsorption equilibria: Na-zeolites had the highest data adsorption equilibrium selectivity for CO2 and N2 or CO2 and CH4, followed by Li-zeolites, which only had a strong adsorption potential of CO2; K-zeolites with high SCO2/N2 and SCH4/N2, based on the strong adsorption of CO2 and CH4. We conclude that the adsorption potential order was K-zeolites > Na-zeolites > Li-zeolites, so the bigger ions had a stronger affinity.
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INTERNATIONAL JOURNAL OF MULTIPHASE FLOW
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2020
·
IF 3.083
Xiaofei Xu,Victus Kordorwu,Zhi Li,Fengxia Liu,Wei Wei,Zhijun Liu
Single CO 2 bubbles rising in quiescent viscoelastic polyacrylamide (PAA) aqueous solutions of different weight percentages (wt. %) were studied to obtain insight into the impact of fluid elasticity on the rising dynamics of dissolving bubbles. A random abrupt fall and rise in velocity was observed as the bubble velocity gradually and progressively decreased throughout the journey. This is the first time this observation is reported. In the most viscoelastic medium in which this phenomenon occurred, CO 2 bubbles decreased in diameter by at least 20% over 1m of height. Mass transfer analysis of the system indicated significant reduction of mass transfer coefficient with increase in weight percentage of the polymer solution. Comparison of experimental mass transfer coefficients with predictions for mobile and immobile gas-liquid interfaces were consistent with theoretical predictions from Higbie's and Frössling's equations respectively. The rising dynamics was correlated using dimensional analysis, and the prediction by a developed empirical correlation considering the combined effect of fluid elasticity and shear-thinning property showed a satisfactory agreement with experimental data in all liquids studied.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Feng Zhao,Yimin Deng,Miyi Li,Can Lv,Tejraj M. Aminabhavi,Ozge Yuksel Orhan,Helei Liu
The CO 2 desorption in amine-based carbon capture processing is accompanied by significant energy consumption, accounting nearly 70% of energy requirements of the entire process. Electrochemical CO 2 capture and release are promising technologies to reduce the energy consumption. The characteristics and CO 2 desorption performance of QH 2 (Tiron) in tertiary amine systems are investigated in this research. The reducing ability of Q (Oxidized QH 2 ) was improved by modifying the electrode to achieve low-energy electrochemical desorption. The CO 2 electrochemical desorption achieved low-energy CO 2 desorption of 0.7 GJ ton −1 CO 2 against over 2.4 GJ ton −1 in a conventional and mature MEA-based system.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Guiming Xie,Xingyang Bai,Yanrui Niu,Runduo Zhang,Jian Liu,Qingyuan Yang,Zhou-Jun Wang
Making use of novel materials to develop efficient catalysts is one of the research hotspots for CO2 hydrogenation to methanol. Herein, UiO-66, a typical Zr-MOF, was modified by ethylene diamine tetraacetic acid (EDTA) to serve as a substrate for the synthesis of AuCu bimetallic catalysts. The resultant AuCu@UiO-66-EDTA catalyst exhibited a superior methanol production rate, which delivered a high space-time yield of methanol (3.34 gMeOH gmetal–1 h–1) at 250 °C and 3.0 MPa. The EDTA modification was found to effectively confine AuCu nanoparticles inside the framework of MOFs, which significantly reduced the metal particle size and enriched the oxygen vacancy concentration. As a consequence, more active sites were generated for methanol synthesis. Moreover, the AuCu@UiO-66-EDTA catalyst yielded more favorable reaction intermediates that could be converted to methanol at a faster rate. This work develops unique MOFs-encapsulated bimetallic catalysts and illuminates the positive effect of confinement.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Yuting Li,Dandan Wang,Yuqin Ma,Fangbin Liu,Hongji Li,Qigming Xu,Haijiao Xie
The reduction of carbon dioxide (CO2) using electrochemical methods is one of the ways to achieve carbon recycling, as the increase in carbon dioxide emissions causes environmental problems. Single-atom dispersed Ni-NC site catalysts have emerged as effective electrocatalysts for the reduction of CO2 to CO. Using ZIF-8 as a carrier, we aim to design a high-performance single nickel-site catalyst by elucidating the structure evolution of NiNx sites during thermal activation as well as other key external factors such as the carbon particle size and nickel content. The pyridine N active sites generated after calcination have higher activity and CO selectivity. The catalyst achieved up to 99.6% CO generation at −0.88 V vs. RHE, and is one of the best catalysts for the reduction of CO2 to CO. This work demonstrates an effective method for designing efficient electrochemical CO2 reduction catalysts by tuning the surface structure of single-atom anchored carriers.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Changhai Lu,Xinru Li,Juan Li,Liang Mao,Mingshan Zhu,Qin Chen,Long Wen,Baojun Li,Tuan Guo,Zaizhu Lou
Plasmonic semiconductors with both features of metals and semiconductors are expected materials for solar light harvesting. Here, plasmonic semiconductor heterostructures were constructed by coupling pyroelectric black phosphorus (BP) and plasmonic tungsten oxides (WO) as photocatalyst for CO 2 reduction. Intriguingly, under visible and near-infrared (NIR) light irradiation, the plasmonic BP/WO heterostructures with optimal composition exhibit high-selective 26.1 μmol g -1 h −1 CO generation (98 %), which is 7- and 17-fold higher than those of plasmonic WO and pyroelectric BP, respectively. The interface bonds (P-O-W) were detected by FTIR spectra and demonstrated by density functional theory (DFT) calculations as dominant channels for electron transfer from BP to WO. Plasmonic thermal effect of WO can increase the local temperature to 86 °C under visible and NIR light irradiation, triggering pyroelectric effect of BP and generating pyroelectric carriers, which enhance the electron transfer from BP to WO. Therefore, continuous electron injection from pyroelectric BP to WO enhances surface plasmon resonance for high-selective CO 2 reduction. This work provides clear proofs to demonstrate that constructing pyroelectric effect on plasmonic heterostructures is one useful strategy to promote NIR-harvesting for artificial photosynthesis.
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Molecular Catalysis
·
2025
·
IF 4.9
Lu Ren,Bin Wang,Yueli Wen,Maohong Fan,Zhaoxiong Huang,Wenxuan Li,Wei Huang,Jing Li,Jianping Guo
Acid-base synergistic effect is crucial in adjusting the catalytic performance of CO 2 hydrogenation to methanol, an efficient CO 2 emission reduction and carbon recycle strategy. Two MOFs-derived catalysts (CZ-MIL, CA-ZIF) with opposite acid-base properties were tailored by using MIL-68 (Al) and ZIF-8 (Zn) as precursors, and the above two MOFs precursors were hybridized (C-ZAx) to control the acid-base property of the catalyst. C-ZA0.6 (molar ratio of MIL-68 (Al) to ZIF-8 (Zn)=0.6) exhibits a promising catalytic performance with CO 2 conversion of 8.9 %, methanol selectivity of 61.85 %, and STY of 117.02 mg mL −1 ·h −1 at 4 MPa and 523 K. Combined with comprehensive analysis, it is found that methanol selectivity is closely related to weak acid sites arising from the residual skeleton of MIL-68. Acid-base synergy facilitates the hydrogenation of CO 2 to methanol. The basic sites are responsible for adsorbing and activating CO 2 , and the acidic site helps to stabilize CO* and facilitate the further hydrogenation to methanol. This work provides a new idea and feasible method for enhancing the catalytic performance of CO 2 hydrogenation to methanol.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Xiting Tao,Chunyan Zhang,Zhiming Yang,Chao Yao,Xiazhang Li
The conversion of carbon dioxide and water into fuels through artificial photosynthesis is of great significance for achieving carbon neutrality. However, this reaction faces great challenge due to the sluggish kinetics. Herein, high-entropy spinel (NiFeMnCoCu) 3 O 4 nanoparticles supported on palygorskite (Pal) were synthesized using a facile sol-gel method, and the composite was employed for photocatalytic CO 2 reduction coupled with biomass-derived 5-hydroxymethylfurfural (HMF) oxidation. The hydrochloric acid-modified Pal (H-Pal) facilitated the generation of high concentrations of oxygen vacancies in (NiFeMnCoCu) 3 O 4 , inducing a localized surface plasmon resonance (LSPR) effect, expanding the light absorption range to the near-infrared region and releasing high-energy hot electrons, thereby enhancing the photocatalyst's photothermal conversion capability. The HMF oxidation along with dehydrogenation addressed the issue of slow kinetics while harnessing the potential of biomass resources. Moreover, the high concentration of oxygen vacancies significantly improved the separation efficiency of charge carriers, favoring the enhanced photocatalytic CO 2 reduction and HMF oxidation ability of the (NiFeMnCoCu) 3 O 4 /H-Pal composite. Current study provides a novel strategy for the conversion of CO 2 and the high-value utilization of biomass.
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