CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Guangjun Ji,Cunyao Li,Benhan Fan,Guoqing Wang,Zhao Sun,Miao Jiang,Lei Ma,Li Yan,Yunjie Ding
Rational designing the structure of catalysts is an effective but challenging way to optimize catalytic performance for target reaction, which is especially significative in the field of single site catalysts. In this work, a kind of single Rh catalysts for heterogeneous hydroformylation of olefins with CO 2 as substituted carbonyl sources was designed. By simply doping N sites surround Rh P active sites, Rh 1 /POPs-P&N were endowed with better catalytic performance even than homogeneous Rh P complex catalysts. Our study showed that the fine fabricated skeleton structure of Rh 1 /POPs-P&N could endow the N sites with function promotion effect on the adjacent Rh P active sites to different degrees. Consequently, the Rh 1 / m -POP-PPh 3 &PMPD, which formed more HRh(CO) 2 (P) 2 species during the reaction, exhibited the highest yield of aldehydes (conversion of 89 %, selectivity toward aldehydes of 87.1 %, l/b ratio of 13.1), good stability (5 recycling runs without activity loss) and extensive substrate applicability (12 kinds of olefins) in heterogeneous hydroformylation of olefins with CO 2 , surpassing all homogeneous and heterogeneous catalysts that only contain Rh P sites (Table 5). Multiple characterization techniques (EXAFS, STEM, in-situ FTIR etc. ) were employed to get insights into this effective strategy to rationally design efficient single site catalysts.
研究领域:
催化
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材料科学
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化学反应工程
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无机化学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS SCIENCE FORUM
·
2024
·
IF 0
Ya Ya Wang,Xin Jin
To alleviate the environmental problems caused by the excessive emission of CO2, this study designed and synthesized a binary organocatalytic system based on urea-based hydrogen bond donors and polyether ionic liquids based on a cycloaddition reaction that converts CO2 and small-molecule epoxides into cyclic carbonates with high industrial application value. The binary system is based on a polyether ionic liquid, introducing an organic base (to trap and activate CO2), hydrogen bond donor (to activate the epoxide), and nucleophilic reagent unit (to help open the ring of epoxides), with a variety of active sites. In this paper, the effects of the hydrogen bond donor as well as polyether ionic liquids structure on the activity of the binary system were investigated, the optimal HBD/Lewis base binary catalytic system was established, and the cycle life of this binary system was tested.
研究领域:
化学
·
环境科学
·
催化材料
✓ 已验证
DOI
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Sifan Bao,Xudong Zheng,Zihuai Xu,Zhouzhou Yang,Wei Sun,Jinfeng Mei,Jian Rong,Zhongyu Li
Carbon aerogel is limited in its application in CO 2 capture due to its poor surface properties. Heteroatom doping is conducive to the adsorption of CO 2 by biochar. Therefore, by in-situ synthesis of nitrogen-doped carbon nanotubes on BC, Ni/N co-doped cellulose carbon aerogel was synthesized, and the results showed excellent adsorption capacity and reversible adsorption/desorption properties. The synthesis of nitrogen-doped carbon nanotubes made the material realize N doping and provided more adsorption sites for CO 2 adsorption. When Ni is dispersed in the material, it not only increases the carbon dioxide adsorption sites but also enhances the thermal stability and cycling performance of the composite material. Meanwhile, the coordination effect between nickel and nitrogen further enhances the capture capacity of carbon dioxide. Ultimately, the adsorption capacity of the modified biochar reached 4.89 mmol/g, and it also has good recycling performance. The unique co-doping design strategy reduces the dependence of traditional carbon materials on surface area when adsorbing CO 2 , providing a new direction for the modification of carbon materials.
研究领域:
环境科学
·
材料科学
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化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Science
·
2022
·Vol. 15
·期 8
·3494-3502
·
IF 39.714
Lianpeng Song,Zhong Liang,Mingzi Sun,Bolong Huang,Yaping Du
The selectivity in the electrocatalysis of carbon dioxide reduction reaction (CO2RR) has attracted tremendous attention but still faces a great challenge. Constructing an interface has become an advanced strategy to effectively modulate electroactivity and selectivity. Herein, we report the synthesis of a CeO2/Bi3NbO7 fibrous tubular structure through a simple electrospinning method, which has shown a much-improved selectivity of 84.73% towards formic acid with remarkable durability in the CO2RR. Theoretical calculations have demonstrated that the construction interface has supplied highly electroactive regions with efficient electron transfer, which not only improves the adsorption of key adsorbates but also alleviates the reaction energy barriers. The modulation induced by the interface enables the high selectivity and yield of HCOOH. This work has supplied a novel and advanced strategy to utilize the interfacial effect in developing superior CO2RR electrocatalysts in the future.
研究领域:
材料科学
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电化学
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催化
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环境科学
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Xiaowen Su,Shan Wu,Xiaoxing Long,Yan Shi,Qi Pan,Jixin Su
Preventing climate change and achieving carbon neutralization depend on strengthening the carbon cycle in industry and limiting carbon emissions to ambient air. Our aim is to reduce CO 2 to valuable CO by gas-solid photo-catalytic reduction under sunlight. We prepared catalysts by one-step synthesis with graphene oxide (GO) and ZnO, surface modified with a monolayer of sulfonated cobalt phthalocyanine (CoPcS), which were calcined to obtain photocatalyst samples containing Co(II), ZnO and reduced graphene oxide (rGO). Results of TEM, SEM-EDS, XRD, XPS, PL and ESR revealed that the photocatalyst samples possessed a hybrid layer microstructure, heterojunction, and excellent electron-hole pair separation. Evaluation of the photocatalytic reduction reactivity showed that CO selectivity reached 96.2–99.0% and top CO yield was 26.15 µmol.g −1 .h −1 .
研究领域:
环境科学
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材料科学
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化学工程
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光化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jie Qi,Jian Lan,Shaoyang Liu,Li Tong,Yuzhe Li,Na Wang,Zheng Zhang,Hongsheng Lu
One of the challenge in the remediation of contaminated soil by solvent washing is the retrieval of total petroleum hydrocarbons (TPH) and solvents. Herein, a CO 2 switchable hydrophobic low temperature transition mixture ([DPA][EL]) composed of ethyl lactate (EL) and dipropylamine (DPA) is proposed, accompanied by a proof-of-concept for contaminated soil washing. The path and energy of hydrogen bond interactions in [DPA][EL] were revealed by the quantum chemical calculation using the quantum theory of atoms in molecule. [DPA][EL] achieved a thorough CO 2 -induced polarity and hydrophobicity transition undergoing an incomplete CO 2 absorption that results in the partial formation of carbonate and carbamate. [DPA][EL] was regenerated after the removal of CO 2 by heating at 85 °C for 2 min. Thanks to this peculiarity, the time required for hydrophobicity transition was 197 times shorter than that of the typical CO 2 switchable hydrophobic solvent, N,N -dimethylcyclohexylamine. The polarity of [DPA][EL], quantified by the normalized polarity energy, increased by 346.69 % after the introduction of CO 2 because of the synergistic effect of water. This ultra-sensitive transition behavior intensified the CO 2 -induced separation of oily compounds, e.g., kerosene and crude oil. The conceptual usage of [DPA][EL] in the contaminated soil washing was demonstrated. The TPH content of contaminated soil decrease from 8.27 % to 0.31 % by [DPA][EL] washing through tailoring the molar ratio of DPA to EL in [DPA][EL], temperature, and [DPA][EL] to contaminated soil ratio (L/S, mL/g). [DPA][EL] whose composition possesses different polarities compensated for the poor solubility of single solvents towards TPH, thereby improving the washing efficiency of contaminated soil. Afterwards, TPH was separated upon triggered by CO 2 /water in 2 min, and 91.33 % of [DPA][EL] was subsequently regenerated at 85 °C in 2 min.
研究领域:
环境科学
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化学工程
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土壤修复
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Zhong Changyin,Yang Yifei,Chen Jun,Feng Bomin,Wang Hongbing,Yao Yunxi
CO 2 methanation is regarded as an efficient method for upgrading CO 2 to fuels and reducing environmental impacts of greenhouse gas emission. In this study, we developed Ni/ La 2 O 2 CO 3 low temperature CO 2 methanation catalysts by tuning the metal-support interaction via changing the morphology of catalyst supports. La 2 O 2 CO 3 supports with various morphologies including nanotriangles (La 2 O 2 CO 3 -T), nanorods (La 2 O 2 CO 3 -R), and nanoparticles (La 2 O 2 CO 3 -P), were synthesized as the supports of Ni catalysts for CO 2 methanation reaction. The CO 2 methanation performance of the synthesized Ni/La 2 O 2 CO 3 catalysts was found to be markedly superior to that of conventional Ni/SiO 2 catalysts with the following orders: Ni/La 2 O 2 CO 3 -T > Ni/La 2 O 2 CO 3 -R > Ni/La 2 O 2 CO 3 -P > Ni/SiO 2 . In the comparative characterization of Ni/La 2 O 2 CO 3 catalysts with various morphologies, TEM and H 2 -TPR results reveal that the Ni/La 2 O 2 CO 3 -T catalysts exhibit better dispersion of Ni nanoparticles and higher reducibility. Moreover, X-ray photoelectron spectroscopy (XPS), O 2 and H 2 temperature programmed desorption (O 2 -TPD, H 2 -TPD) results indicate that the Ni/La 2 O 2 CO 3 -T catalysts possess a lower oxygen vacancy formation energy leading to a higher concentration of interfacial oxygen vacancies, which enhances the adsorption hydrogen at these interfacial oxygen vacancy sites. CO 2 -TPD results further reveal that Ni/La 2 O 2 CO 3 -T catalysts own higher concentration of medium basic sites, which promote the adsorption and activation of CO 2 . Consequently, Ni/La 2 O 2 CO 3 -T catalysts demonstrate superior low-temperature CO 2 methanation activity by hydrogenation of CO 2 adsorbed as surface carbonates on the La 2 O 2 CO 3 surfaces with hydrogen spilled over from the Ni surfaces via the interfacial oxygen vacancies to the catalyst support. Graphical Abstract
研究领域:
催化
·
材料科学
·
环境化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Yafei Guo,Changhai Li,Shouxiang Lu,Chuanwen Zhao
K 2 CO 3 supported on activated carbon (K 2 CO 3 /AC) shows promise as a potential candidate for removing low-concentration CO 2 from environmental control and life support systems (ECLSS). However, K 2 CO 3 /AC would suffer a decreased CO 2 sorption capacity due to sorbent deactivation in acid impurities such as SO 2 and NO 2 . To solve this problem, water vapor pretreatment, KOH addition and polyethyleneimine (PEI) modification were proposed as efficacious means for improving its CO 2 sorption capacity and mitigating the sorbent deactivation in these acid impurities. CO 2 sorption performances of the pretreated and modified sorbents were evaluated in a fixed-bed reactor under simulated ECLSS conditions of 20 °C, 1.0% CO 2 , 2.0% H 2 O, 30 ppm SO 2 , 20 ppm NO 2 and balanced N 2 . The mechanisms for sorbent deactivation inhibition by water vapor pretreatment, KOH addition and PEI modification were revealed by N 2 adsorption-desorption, X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM) and Fourier transform infrared spectroscopy (FT-IR). Effects of water vapor pretreatment duration, KOH addition and PEI loading on sorbent deactivation inhibition performances were demonstrated. Furthermore, the long-term working stabilities of the pretreated and modified sorbents in impurities were evaluated. The results will provide fundamental support on practical application of K 2 CO 3 /AC for low-concentration CO 2 removal in ECLSS.
研究领域:
环境控制与生命支持系统
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气体吸附
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材料化学
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空气净化技术
·
二氧化碳捕集
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Peng Li,Chao Ma,Ning Li,Chi Tang,Zhaolin Lv,Zhenjie Gu,Zhihua Qiao,Chongli Zhong
Metal-organic framework (MOF) membranes have demonstrated significant potential in replacing traditional polymer membranes for gas separation. However, synergistically enhancing gas permeance and selectivity remains challenging in MOF membrane design, particularly when framework pore apertures surpass gas kinetic diameters. Here, an innovative strategy is reported for engineering ultrathin ZIF-8 membranes with chemical adsorption sites via polymer bidirectional induction. The polyethyleneimine (PEI)-Zn 2+ interface layer facilitated the formation of ultrathin ZIF-8 membranes (~78.4 nm) by guiding small-sized crystal growth. Meanwhile, the competitive coordination of PEI with 2-methylimidazole induced the pendant of partially coordinated ligands in the ZIF-8 cavity to form chemisorption sites. This structural alteration enabled the in-situ chemical adsorption of CO 2 in the cavity of ZIF-8, thus contracting the window apertures and enhancing the molecular sieving efficiency. As a result, the ultrathin ZIF-8 membrane exhibited an excellent H 2 /CO 2 ideal selectivity of 34.2 with a remarkable H 2 permeance of 7143.6 GPU in single-gas tests, outperforming other reported ZIF-8 membranes. During mixed-gas H 2 /CO 2 testing, the in situ structural changes demonstrated robust pressure-performance stability and long-term gas separation capability. This work advances the development of ZIF-8 membranes for efficient separation of H 2 /CO 2 , and offers a feasible design principle and theoretical guidance for MOF-based gas separation membranes.
研究领域:
材料科学
·
化学工程
·
膜技术
·
气体分离
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 23
·期 3
·2005-2014
·
IF 3.43
Haibin Gou,Xifei Ma,Qian Su,Lei Liu,Ting Ying,Wei Qian,Li Dong,Weiguo Cheng
The development of metal-free, high effective and recyclable catalysts plays a pivotal role in transforming CO2 into high value-added products such as cyclic carbonates. In this paper, we introduced the hydrogen bond donor (HBD) groups into poly(ionic liquid)s via free radical polymerization, which successfully combined the HBD and ionic liquids (ILs) into one heterogeneous catalyst. The HBD could synergistically activate epoxides with hydroxyl functionalized ionic liquids and efficiently catalyze the cycloaddition of CO2 into cyclic carbonates. The yield of propylene carbonate (PC) reached 94% (at 105 °C, 2 MPa CO2, 3 h), which far exceeded poly(ionic liquid)s without HBDs functionalization (PC yield 72%), and even approached bulk ionic liquids (PC yield 95%). Moreover, HBD-functionalized poly(ionic liquid)s (HPILs) exhibited excellent recyclability after five runs and afforded wide substrate scope. According to the experimental results, 1H NMR spectra and density functional theory (DFT) calculations showed 2-hydroxyethyl methacrylate (HEMA) and the hydroxyl of ILs would form strong H-bonds with epoxides contributing to the ring-opening process of epoxides, and a possible HBD and nucleophilic anion synergistically catalytic mechanism was proposed. The method herein paved a brand new way for green technology and utilization of poly(ionic liquid)s.
研究领域:
材料科学
·
化学工程
·
催化
·
绿色化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Longkai Pan,Minggang Zhang,Hui Mei,Li Yao,Zhipeng Jin,Hongxia Liu,Shixiang Zhou,Ziyi Yao,Gangqiang Zhu,Laifei Cheng,Litong Zhang
Use of 3D photocatalytic reactor has been widely explored for development of efficient photocatalytic systems. In the present study, a bionic palisade cells BiOBr/Sr 2 Nb 2 O 7 /Al 6 Si 2 O 13 photocatalytic reactor with high strength was prepared through combination of 3D printing technology and solvothermal method. The carefully designed and optimized bionic palisade cell structure exhibited a periodic porous structure with high surface area. The controllable periodic structure effectively regulated the internal photon transfer and mass transfer. Photon transfer ensured that light is fully scattered within the structure, which improved light utilization. High mass transfer ensured smooth flow of reactant inside the structure, which increased reactant adsorption on the surface of photocatalysts. The interface electric field of the BiOBr/Sr 2 Nb 2 O 7 p-n heterojunction effectively separated the photogenerated electrons and holes. The BOB/SNO/ASO structure had high photocatalytic CO 2 reduction performance under the simulated sunlight. The CO yield for the reaction was 13.68 μmol/g/h, whereas that of CH 4 yield was 6.37 μmol/g/h. Therefore, the findings of the present study provide a basis for design and preparation of high-performance 3D photocatalytic reactors.
研究领域:
材料科学
·
环境科学
·
化学工程
·
光催化
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Yusheng Qiu,Shuzhuang Sun
The activity and selectivity of catalytic reactions are profoundly influenced by metal–support interactions. The strong metal–support interaction (SMSI) plays a critical role in selectively driving the conversion of CO2 toward CO instead of CH4 in Ni-based catalytic systems. Moreover, the dispersion of active species governs the population of accessible reaction sites, thereby enhancing catalytic activity. In this work, highly efficient SMSI was successfully constructed via steam aging post-treatment over CeO2–Al2O3 nanocrystalline loaded Ni catalysts (NiCeAl). Remarkably, the NiCeAl–H2O catalyst achieves ∼50% CO2 conversion with 90% CO selectivity at 600 °C, representing a dramatic improvement over the untreated NiCeAl catalyst (23% CO2 conversion with ∼92% CO selectivity). Furthermore, the steam-treated catalyst demonstrates superior stability in prolonged CO2 hydrogenation tests, maintaining its performance with only a ∼4% conversion decrease over 10 h of continuous operation. In situ diffuse reflectance infrared Fourier transform spectroscopy analysis revealed that CO2 chemisorbs on the catalyst surface to form bidentate carbonates, which undergo sequential hydrogenation to form formate intermediates. These formate species subsequently decompose catalytically to produce CO, with the enhanced MSI in NiCeAl–H2O facilitating optimal CO desorption kinetics, thereby promoting superior reverse water–gas shift activity.
研究领域:
催化
·
材料科学
·
化学工程
·
环境化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）