JOURNAL OF NANOPARTICLE RESEARCH
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2020
·Vol. 22
·期 7
·1-9
·
IF 2.132
Ren Wen,Wei Zhenzhen,Xia Xiaoxiao,Hong Zhiwei,Li Song
Metal-organic frameworks (MOFs) have been recognized as promising adsorbents for carbon capture due to their ultrahigh surface areas and tunable properties. However, a majority of MOFs have strict requirements for preparation and high mass transfer resistance that limits the gas separation time. In order to improve the applicability of MOFs to practical applications, herein, we reported an experimental approach to prepare structured CuBTC/graphene aerogel (GA) composites using ionic liquid (IL) additives (CuBTC/GA-IL) at room temperature for CO 2 capture. The material was characterized by powder X-ray diffraction (PXRD), scanning electron microscopy (SEM), specific surface area analysis, and CO 2 adsorption tests. It was demonstrated that CuBTC/GA-IL exhibited the higher CO 2 uptake than CuBTC/GA prepared without IL additives. Besides, the breakthrough experiments have shown that CuBTC/GA-IL exhibited the lower mass transfer resistance compared with CuBTC-IL and good cyclability. The effective approach of fabricating CuBTC into GA using IL additives to improve CO 2 adsorption in this study may be extensively applied for other MOF-based composites.
Graphical abstract
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Science China-Chemistry
·
2020
·Vol. 63
·期 12
·1721-1726
·
IF 6.356
He Chaohua,Chen Sijia,Long Ran,Song Li,Xiong Yujie
The sharp rise of CO 2 in the atmosphere has become a potential threat to global climate, which results from the massive utilization of fossil fuel since the industry revolution. CO 2 electroreduction provides us a new possibility of utilizing CO 2 as a carbon feedstock for fuel and commercial chemicals generation. In this article, a new method is developed for synthesizing CuInS2 hollow nanostructures through the Kirkendall effect. The CuInS 2 hollow nanostructures exhibit excellent catalytic activity for electrochemical reduction of CO 2 with particular high selectivity, achieving high faradaic efficiency for HCOOH of 72.8% at −0.7 V. To elucidate the mechanisms, operando electrochemical Raman spectroscopy is employed to examine the CO2 reduction process. This work provides new insights into the design of hollow nanostructures toward electrocatalytic CO2 conversion and offers us an effective and reliable way for real-time investigation of electrochemical CO2 reduction reaction processes.
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Bingquan Jia,Du Sun,Chengjin Li,Wei Zhao,Heliang Yao,Fangfang Xu,Fuqiang Huang
Metal cyanamides have an organic–inorganic hybrid structure similar to MOFs, which are expected to possess interesting catalytic properties. However, the structural complexity of these compounds sets up a big barrier to realize shape manipulation and further understanding on the structure–activity relationship. Here, we describe seed-mediated colloidal synthesis as a facile approach to obtain Ag2NCN near-monodisperse nanocrystals (NCs: nanorods, nanowires, and nanosheets) and their related CO2 catalytic activity. The control experiment unveiled the prominent role of the anisotropy for quasi-linear [NCN]2– anions in obtaining the desired growth order of different crystal planes. The formic acid production of nearly 20% Faradaic efficiency is observed when the as-prepared Ag2NCN NCs were tested for electrocatalytic CO2 reduction reactions. The exposed (200) planes exhibit evident higher catalytic activity compared to other planes, showing morphology-dependent activity. Our result reveals that the anisotropic structure of ions leads to their preferential growth of the NCs and thus may have greater implications for the shape-controlled synthesis of complex ions containing compounds and their related catalytic activity.
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Small Methods
·
2024
·
IF 10.7
Yajuan Niu,Qinbo Liu,Xu Ou,Yingjie Zhou,Zhe Sun,Feng Yan
Large amounts of small molecule dyes leak into the ecosystems annually in harmful and unsustainable ways. Polymer dyes have attracted much attention because of their high migration resistance, excellent stability, and minimized leakage. However, the complex synthesis process, high cost, and poor degradability hinder their widespread application. Herein, green and sustainable polymer dyes are prepared using natural dye quercetin (Qc) and CO 2 through a one-step process. The CO 2 -sourced polymer dyes show strong migration resistance, high stability, and can be degraded on demand. Additionally, the CO 2 -sourced polymer dyes showed unique responses to Zn 2+ , leading to significantly enhanced fluorescence, highlighting their potential for information encryption/decryption. The CO 2 -sourced polymer dyes can solve the environmental hazards caused by small molecule dye leakage and promote the carbon cycle process. Meanwhile, the one-step synthesis process is expected to achieve sustainable and widespread utilization of CO 2 -sourced polymer dyes.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 31
·15884-15890
·
IF 11.301
Rong Xia,Sheng Zhang,Xinbin Ma,Feng Jiao
Rational design and synthesis of efficient catalysts for electrochemical CO2 reduction is a critical step towards practical CO2 electrolyzer systems. In this work, we report a strategy to tune the catalytic property of a metallic Pd catalyst by coating its surface with a polydiallyldimethyl ammonium (PDDA) polymer layer. The resulting PDDA-functionalized Pd/C catalysts exhibit an enhanced CO faradaic efficiency of ∼93% together with a current density of 300 mA cm−2 at −0.65 V versus reversible hydrogen electrode in comparison to non-functionalized and commercial Pd/C catalysts. X-ray photoelectron spectroscopy analysis reveals that the improvement can be attributed to the electron transfer from the quaternary ammonium groups of PDDA to Pd nanoparticles, weakening the CO binding energy on Pd. The weak CO adsorption on Pd was further confirmed by the CO temperature programmed desorption measurement and operando attenuated total reflection-Fourier-transform infrared analysis. Therefore, the incorporation of electron-donating groups could be an effective strategy to decrease the CO binding energy of a metallic catalyst for a high CO selectivity in CO2 electroreduction.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Weicheng Xu,Bingxu Chen,Xueding Jiang,Feng Xu,Xin Chen,Limin Chen,Junliang Wu,Mingli Fu,Daiqi Ye
The effect of Ca modification on the Ni/ZSM-5 catalyst for efficient toluene oxidation was studied in a plasma-catalytic system. The Ni/ZSM-5 and Ca-Ni/ZSM-5 catalysts were prepared by a wet impregnation method and characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), Pyridine-FTIR spectroscopy and temperature programmed desorption of ammonia (NH 3 -TPD). Among the catalysts tested, the Ca-Ni/ZSM-5 sample showed the best potential for toluene conversion (90.2%) and CO 2 selectivity (70.7%). Pyridine-FTIR spectra and NH 3 -TPD results proved that the introduction of Ca and Ni onto ZSM-5 caused a decrease in the strong and weak acidic sites. In addition, gas chromatography/mass spectrometry (GC-MS) result showed that the Ca-Ni/ZSM-5 catalyst reduced the production of undesirable byproducts (such as p-nitrotoluene and methyl benzoate). Calcium in the Ni/ZSM-5 system influenced the acidity and other surface characteristic of the catalyst, as well as directly impacting the reactive plasma species and the intermediates. Finally, possible reaction mechanisms in the plasma catalysis of toluene were also proposed.
研究领域:
环境催化
·
大气污染控制
·
材料化学
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表面科学
·
等离子体化学
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JOURNAL OF RARE EARTHS
·
2026
·
IF 9.6
Zhichao Chen,Wenchao Wang,Hongzhi Wang,Licheng Liu
Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) to produce value-added methane (CH 4 ) represents a promising approach to achieve carbon recycling and addressing global energy challenges. However, this reaction is currently hindered by limitations in catalytic selectivity and efficiency. Herein, we present a strategy involving strontium (Sr) doping at the A-site of La 2 CuO 4 perovskite (denoted as Sr x -LCO) to regulate surface basicity, thereby significantly enhancing catalytic performance for CO 2 RR toward CH 4 formation. The optimized Sr 0.04 -LCO catalyst achieves a Faradaic efficiency of 68.8% for CH 4 at −1.1 V (vs. RHE), which is significantly higher than that of undoped La 2 CuO 4 (44.1%) and at the top level among public reports. The results indicate that successful Sr doping to the La-site promotes electron transfer through the La−O−Cu linkage, generating a local alkaline microenvironment around the Sr−O sites. This microenvironment enhances CO 2 chemisorption and provides abundant reactive protons (*H). Theoretical calculations further confirm that the localized alkaline region reduces the activation energy barriers for the rate-determining steps (*CO 2 → *COOH and *CO → *COH) and suppresses the competing hydrogen evolution reaction (HER), thereby selectively steering the reaction pathway toward CH 4 formation. This study elucidates the mechanistic role of surface microenvironment modulation in enhancing CO 2 reduction reaction (CO 2 RR) selectivity for lanthanide perovskite, offering new insights for the rational design of high-performance electrocatalysts.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 6
·1830-1845
·
IF 5
Hong Wang,Zhongming Wang,Mingquan Xiao,Zizhong Zhang,Xianzhi Fu,Wenxin Dai
Improving product selectivity is the most important goal for the artificial photosynthesis of CO2 and H2O considering that the adsorption behaviors of reactants may play an important role in the product selectivity of CO2 conversion. In this work, a black In2O3 sample was modified with fluoride anions (F−) as electron donors or amino ions (NH2+) as electron acceptors. F-modified In2O3 provided additional F− and In2+ sites, which promoted H2O to accept more electrons from the material, and exhibited a high selectivity to CH4 of 81.95%. NH2-modified In2O3 caused H2O to donate electrons to the material by constructing a hydrophobic layer, resulting in a high combined selectivity to methanol and carbon monoxide of 87.64%. Based on the two different H2O adsorption behaviors at In2+ sites adjacent to oxygen vacancy defects (VO–In2+) or at In3+ sites, the respective formation of hydrogen ions (H+) or protons (*H) is key to regulating the product selectivity of CO2 reduction. The formation of a confined-space structure of CO2 and its capacity to accept more electrons from the material induced by a higher number of VO–In2+ sites after modification both ensure the proceeding of CO2 reduction. The findings presented in this work add to the understanding of artificial photosynthesis.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Peng Liu,Huiling Liu,Shun Zhang,Jie Wang,Cheng Wang
Electroreduction of carbon dioxide (CO 2 ) into formic acid/formate has been considered as one of the most promising strategies for obtaining value-added fuels and chemical productions. Herein, we present a general method for preparing Bi-based electrocatalysts via in situ reduction of bismuth oxyiodide (BiOI) in CO 2 -saturated electrolyte. The precursors of BiOI nanoplates (P-nanoplates) with thickness of 30–40 nm could be easily obtained and provide a concise model to probe the mechanisms of CO 2 reduction to formate. BiOI nanoplates precursors derived Bi nanosheets (P-nanoplates-Bi) exhibited an excellent performance for CO 2 reduction to formate, achieving Faradaic efficiencies (FEs) over 80% in a wide potential window and a maximum FE approaching of 95% with a current density of 13.3 ± 0.6 mA cm −2 at −0.9 V versus reverse hydrogen electrode (υs. RHE). Such P-nanoplates-Bi nanosheets showed a stable electrocatalytic actitivity during 15 h operation in 0.5 M KHCO 3 aqueous solution. The superior performance is mainly attributed to the two-dimensional (2D) Bi nanosheets, which can increase CO 2 •- adsorption, enlarge active surface area, show better reaction kinetics and provide lower contact resistance with accelerated electron transfer . For comparison, precursors of BiOI plate-like (P-bulk) with doubled thicknesses and ultrathin BiOI with a few nanometers derived Bi catalysts tend to agglomerate and appear as irregular structured Bi nanoparticles during the reaction. Their peak FEs for formate are much lower than those of P-nanoplates derived Bi nanosheets at −0.9 V.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Ge Gao,Wufeng Jiang,Xiaoshan Li,Zhenghong Zhao,Cong Jiang,Cong Luo,Fan Wu,Liqi Zhang
Energy consumption is one of the crucial factors in determining the suitability of the chemical absorbents for capturing carbon dioxide (CO 2 ). Polyamines have attracted increasing attention in recent years because of the existence of several amino functional groups that could effectively capture CO 2 in their molecules. In this work, the structures of seven polyamines with excellent CO 2 capture performance were investigated in relation to reaction rate and the CO 2 absorption heat. A high-precision microcalorimeter was applied to analyze the absorption heat of CO 2 directly, and a parameter defined as the CO 2 quasi-cycle capacity was employed to assess the cyclic capture capacity of CO 2 , absorption rate, and desorption rate. Experimental results revealed that for the selected polyamines, the increase in the ratio of the secondary amino functional group to the primary-one in the molecule leads to a decrease in the CO 2 absorption heat and an increase in the CO 2 cyclic capacity.The ΔH abs of the eight amines give out the order of HMDA (92.22 kJ/mol) > MAPA(90.91 kJ/mol) > AEEA (87.62 kJ/mol) > MEA (86.36 kJ/mol) > TEPA (82.95 k/mol) > AEP (82.36 kJ/mol) > 2MPRZ (77.08 kJ/mol) > PZ (74.41 kJ/mol). The CO 2 quasi-cycle capacity of 2MPZR is about twice that of the MEA. In addition, 2MPRZ was found to be an absorbent with phase change potential. The effective phase change solvent system, 2MPRZ + Triethylene glycol monobutyl ether (TGBE) + H 2 O, was developed in this work. Compared to the 5 M MEA aqueous solution, its sensible heat was reduced by 56.3 %, indicating that 2MPRZ is a promising absorbent.
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FLUID PHASE EQUILIBRIA
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2026
·
IF 2.7
Yufan Ma,Cong Liu,Hongxing Wang,Jie Li,Qingli Qian
The solubilities of CO 2 , H 2 , and CH 4 in 1-ethyl-2-pyrrolidone (NEP) were measured using the isochoric saturation method at 413.15–453.15 K under pressures of 0.45–3.89 MPa (CO 2 ), 4.42–7.64 MPa (H 2 ), and 0.59–3.49 MPa (CH 4 ). The reliability of the apparatus was verified by measuring CO 2 solubility in N-methyl-2-pyrrolidone (NMP) at 323.15–353.15 K. The solubility order in NEP was found to be CO 2 > CH 4 > H 2 . Temperature-dependent Henry’s constants were obtained, and the experimental data were correlated using the Krichevsky–Kasarnovsky equation and the generic Redlich–Kwong (RK) cubic equation of state, with the RK model providing better accuracy. These results offer essential thermodynamic data for describing gas–liquid equilibrium in NEP and support solvent selection and process design in high-temperature CO 2 conversion systems.
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RSC Advances
·
2016
·Vol. 6
·期 38
·32400-32404
·
IF 3.289
Zhen-Feng Diao,Zhi-Hua Zhou,Chun-Xiang Guo,Bing Yu,Liang-Nian He
The synthesis of propylene carbonate (PC) from 1,2-propylene glycol (PG) and CO2 was smoothly performed in a PEG800 (polyethylene glycol)/CO2 biphasic system with K2CO3 as a catalyst and propylene oxide (PO) as a dehydrating agent. In the reaction of PG with CO2, PO presumably removes the water produced, and simultaneously generates more PG, both of which shift the thermodynamic control process and thus accelerate the PC synthesis. The PC yield directly from PG and CO2 reached 78% under relatively mild reaction conditions (4 MPa, 120 °C, 10 h). Notably, no additional by-product was detected in this process, resulting in economic benefits and the ease of workup procedure.
研究领域:
绿色化学
·
二氧化碳利用
·
催化化学
·
有机合成
·
可持续化学
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