Materials Today Sustainability
·
2022
·
IF 7.244
R. Zeng,G. Jin,D. He,L. Zhang,D. Chen,Y. Zhang,L. Zhu,Y. Mei,W. Wu,Y. Luo
Utilizing propane and CO 2 as coreactants to produce syngas (CO/H 2 ) via dry reforming shows several advantages over direct propane dehydrogenation and traditional methane dry reforming . It is of great importance to establish high-efficiency catalytic systems that can break C–C bonds and activate CO 2 simultaneously. Herein, acidic H 2 O 2 was applied to etch LaCoO 3 . Surprisingly, highly dispersed Co 3 O 4 at the edges of support along with high oxygen vacancies were obtained from acidic H 2 O 2 treatment. Furthermore, the treated LaCoO 3 catalyst facilitated the generated intermediates of formate to convert into the desired products. The results showed that acidic H 2 O 2 treated LaCoO 3 catalyst can reach 18% for propane conversion and 35% for CO 2 conversion at 550 °C, showing high catalytic activity . Consequently, the present work provides some ideas for the synthesis of efficient LaCoO 3 catalysts for dry reforming of propane.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2022
·Vol. 15
·期 8
·e202200063
·
IF 9.14
Qing Ji,Xiaoping Chen,Ya-Jun Cheng,Qingyu Dong,Yanbin Shen,Zhaohui Yang,Binjie Hu,Yonggao Xia
Graphical Carbon, the master : Constructed with unique carbon emcoating structure through CO 2 acivation, NbO 2 benefited from an effective and highly conductive carbon network, giving rise to exceptional electrochemical performances in terms of reversible capacities, rate capability, and cyclic stability. As a promising alternative as lithium-ion anode, niobium dioxide appeals to researchers due to high theoretical capacity and good electron conductivity. However, rarely work about NbO 2 based high performance anode is reported. Here, NbO 2 nanoparticles emcoated in continuous carbon matrix is constructed through CO 2 /H 2 coupling treatment. CO 2 activation introduces unique carbon emcoating structure, which builds interconnected electron conductive network with low carbon content. Furthermore, crystallographic phase of NbO 2 is enhanced during H 2 treatment, which increases the lithium storage ability. Electrochemical performance of NbO 2 anodes is significantly improved based on the carbon emcoating structure. A high reversible capacity of 391 mAh g −1 is retained after 350 cycles at 0.2 C. Additionally, at a current density of 1 A g −1 , the reversible capacity reaches 139 mAh g −1 . Compared with conventional NbO 2 /C nanohybrids, the lithium diffusion coefficient of carbon-emcoated sample shows improvement of three orders of magnitude. Moreover, the in situ XRD investigation shows a reversible lithium insertion behaviour with a limited volume change.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2018
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IF 4.908
Jingai Shao,Junjie Zhang,Xiong Zhang,Ye Feng,Han Zhang,Shihong Zhang,Hanping Chen
To enhance the SO 2 adsorption of biochar, CO 2 activation and impregnation with methyldiethanolamine (MDEA) was simultaneously employed to improve its physicochemical characteristics. Furthermore, the effects of the pore structure and nitrogen functionality on SO 2 adsorption were also explored. The results show that after CO 2 activation, the specific surface area of biochar increased from 56.91 m 2 /g to 755.35 m 2 /g, while this figure dropped to 25.54 m 2 /g or even lower after impregnation with MDEA. Although the pore structure of activated biochar was destroyed, the surface nitrogen content of the nitrogen-enriched biochar (with 10% MDEA impregnation) increased from 1.46% to its highest level (7.20%); moreover, as indicated by Fourier Transform Infrared (FTIR) spectroscopy, the nitrogen functional groups introduced on the surface of the nitrogen-enriched biochar were mainly C-N. After 10% MDEA impregnation, the maximum SO 2 adsorption capacity increased from 57.8 mg/g to 156.2 mg/g. Changes to physical and chemical properties in the nitrogen-enriched biochar indicate that the nitrogen functional groups on the surface are more important than the pore structure for SO 2 adsorption at 393 K, and that the dominant nitrogen species are quaternary nitrogen.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yongxiao Tuo,Wanli Liu,Qing Lu,Xingzhao Wang,Jiabing Luo,Shutao Wang,Yan Zhou,Min Wang,Xiaohui Sun,Xiang Feng,Mingbo Wu,De Chen,Jun Zhang
The most difficulty of efficient CO 2 electroreduction lies in the activation step that turns CO 2 into the CO 2 − radicals or other intermediates that can be further converted. To overcome this bottleneck, many efforts have been devoted to develop electrocatalysts to lower the overpotential of CO 2 activation, but they inevitably involve complicated or/and unscalable synthesis methods. Here we reported that the SO 4 2− ion modified metal foils, including Zn, Ag, Au and Cu, demonstrated ∼6.5, 1.4, 14 and 2.5 times of CO faradaic efficiency in K 2 SO 4 electrolyte compared to KHCO 3 electrolyte at −1.05 V vs. RHE. According to both experimental and DFT studies, the electron-rich metal-SO 4 adlayer can activate CO 2 by bending the linear molecule of CO 2 through donating electrons to the antibonding orbital of CO 2 , thus facilitating the formation of key intermediate *CO 2 − . Moreover, the adsorption of H + on metal sites is restrained by the metal-SO 4 adlayer, leading to a suppressed H 2 evolution activity. From a broader perspective, many catalysts can benefit from this approach to achieve more efficient CO 2 electrochemical reduction.
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 48
·18942-18951
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IF 8.262
Feng Qian,Xiangdong Zhu,Yuchen Liu,Shilai Hao,Zhiyong Jason Ren,Bin Gao,Ruilong Zong,Shicheng Zhang,Jianmin Chen
Magnetic carbon composites (MCs) have received great interest in areas such as environmental remediation, catalyst supports and carriers for drug delivery systems. In order to improve the porosity of the MCs, the catalytic mechanism of iron salts during CO2 activation of hydrochar was systematically investigated using a suite of methods including Mössbauer spectroscopy, on-line pyrolysis gases and porosity analysis. Fe3O4 and superparamagnetic α-Fe2O3(s), pyrolysis products of iron salts, were found to promote the reaction between carbon and CO2 gas, leading to a decrease in the activation temperature that is required for optimal porosity. However, the reduction reaction between iron oxide and carbon was completely inhibited by CO2 gas. FeCl3 enhanced the thermal cracking of hydrochar and increased the porosity of the MCs in terms of an improvement of the amount of H2, namely the pore-creating effect. However, other iron salts showed adverse effects, due to their inhibition effects on the thermal cracking of hydrochar. The MCs with excellent porosities showed high adsorption capacities for pharmaceuticals and personal care products (PPCPs), and were negatively correlated with the melting points of the PPCPs. The findings from this work can guide the production of novel MCs for maximum removal performance of organic pollutants from the environment.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Zhi-Wen Wang,Qiang Wan,Ying-Zhang Shi,Huan Wang,Yue-Yue Kang,Shu-Ying Zhu,Sen Lin,Ling Wu
Ultrathin TiO 2 nanosheet (NST) with abundant Ti 3+ sites is developed as a photocatalyst which exhibits a high yield (147.2 μmol g −1 h −1 ) and selectivity (96.8%) for CO 2 to CH 4 . The results of in situ FTIR, in situ EPR and density functional theory (DFT) calculation suggest that CO 2 would be selectively activated on NST surface via forming the bridging Ti···CO 2 − ···Ti coordination species which not only lowers the activation energy barrier, but also determines the selectivity of CH 4 . Additionally, NST with the better separation and transfer ability for photogenerated electrons-holes can fleetly supply the electrons to CO 2 molecules for high efficiently producing CH 4 via the Ti-C coordination bond. Finally, a possible mechanism of the synergistic effect about coordination-activation and photocatalysis is discussed at a molecule level. This work would offer a perspective for designing an effective photocatalyst and tailoring the selectivity of products by coordination activation.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
DOI
高影响因子
Small
·
2023
·
IF 13.3
Kai Zhang,Cuiping Xu,Xingjian Zhang,Zhiyi Huang,Qixiang Pian,Kunhong Che,Xiaokun Cui,Yueru Hu,Yimin Xuan
The chemical inertness of CO 2 molecules makes their adsorption and activation on a catalyst surface one of the key challenges in recycling CO 2 into chemical fuels. However, the traditional template synthesis and chemical modification strategies used to tackle this problem face severe structural collapse and modifier deactivation issues during the often-needed post-processing procedure. Herein, a CO 2 self-selective hydrothermal growth strategy is proposed for the synthesis of CeO 2 octahedral nanocrystals that participate in strong physicochemical interactions with CO 2 molecules. The intense affinity for CO 2 molecules persists during successive high-temperature treatments required for Ni deposition. This demonstrates the excellent structural heredity of the CO 2 self-selective CeO 2 nanocrystals, which leads to an outstanding photothermal CH 4 productivity exceeding 9 mmol h -1 m cat -2 and an impressive selectivity of >99%. The excellent performance is correlated with the abundant oxygen vacancies and hydroxyl species on the CeO 2 surface, which create many frustrated Lewis-pair active sites, and the strong interaction between Ni and CeO 2 that promotes the dissociation of H 2 molecules and the spillover of H atoms, thereby greatly benefitting the photothermal CO 2 methanation reaction. This self-selective hydrothermal growth strategy represents a new pathway for the development of effective catalysts for targeted chemical reactions.
研究领域:
材料科学
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催化化学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 7
·1799-1812
·
IF 5.934
Xiaosong Hu,Chaoyue Zhao,Qingxin Guan,Xin Hu,Wei Li,Jun Chen
The chemical transformation of CO2 not only mitigates CO2 released into the atmosphere but also produces fuels and chemicals with important additional value. The activation of stable CO2 molecules is the key difficulty for the efficient conversion of CO2. Herein, we designed a ternary catalyst containing Cu, ZnO, and CeOx and dispersed them in SBA-15 using incipient wetness impregnation. Interestingly, the catalytic performances were improved greatly when the related active components were dispersed inside and outside the pore channels of SBA-15 using the incipient wetness impregnation method. Methanol and CO were controllably produced on the interface of Cu and metal oxides (ZnO and CeOx) due to the synergistic effects between the three active components. The metal oxides play a more important role in CO2 conversion as well as the product selectivity compared to Cu. CeO2 is more efficient than ZnO in promoting the dispersion of Cu nanoparticles and methanol generation. The suitable pore channels of SBA-15 promote the mass transfer and heat transfer while the high specific surface area is favorable to the dispersion of active components, which will facilitate the production of methanol and CO. After continuous hydrogenation evaluation for 100 h, the catalytic performance of the catalyst was still very stable. This work provides a viable strategy to prepare a supported catalyst with highly dispersed active sites, and the catalyst exhibits an efficient catalytic effect on producing methanol and CO.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2021
·Vol. 5
·期 24
·6449-6459
·
IF 6.367
Zhige Zhang,Guofeng Zhao,Han Bing,Jiawei Zhong,Haoran Yuan,Jun Xie,Yong Chen
The efficient utilization of renewable biogas has attracted ever-increasing interest in the past few decades. Ni–Ce1−xZrxO2 supported on monolithic SiC-F (named Ni–Ce1−xZrxO2/SiC-F) is developed and applied in biogas reforming. Monolithic Ni–Ce1−xZrxO2/SiC-F catalysts were comprehensively characterized by ICP-AES, XRD, SEM, HR-TEM, CO2-TPD, etc. The promotional roles of Ce1−xZrxO2 in coke elimination as well as CO2 activation were deeply analyzed via in situ CH4-TPSR/CO2-TPO and in situ H2-TPR/CO2-TPSR. Ni–Ce1−xZrxO2/SiC-F exhibits satisfactory catalytic activity and ability to inhibit sintering and coke-deposition due to (a) the homogeneous dispersion of Ni nanoparticles (NPs) and (b) the strong interaction between Ce1−xZrxO2 solid solutions and Ni NPs. At 900 °C and a weight hourly space velocity (WHSV) of 24 000 mL gcat−1 h−1, an excellent CH4/CO2 conversion of 90/92% was initially achieved over the Ni–Ce1−xZrxO2/SiC-F catalyst, followed by a slight decrease after 150 h, but remained basically stable for the next 250 h.
研究领域:
催化化学
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能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2023
·Vol. 70
·期 4
·e18349
·
IF 3.7
Youluan Lu,Haonan Wu,Dongna Li,Yi Huang,Huijuan Guo,Tielin Wang,Lijuan Shi,Qun Yi
Porous frustrated Lewis pairs (FLPs) have been demonstrated as cutting-edge heterogeneous catalysts in acidic–basic catalysis, which, yet faces great challenges in synthesis. Herein, we propose a one-step de novo assembly strategy for constructing porous FLPs by capping monodentate ionic liquids (ILs) on metal clusters during the synthesis of metal–organic frameworks (MOFs). The capping of ILs makes adjacent metal sites on MOFs transforming to coordinatively-unsaturated metal Lewis acids, producing FLPs containing Lewis basic Cl − ions from ILs and metal sites. The distribution of ILs on the framework of MOFs endows the catalysts with large surface areas (up to 2125 m 2 g −1 ), open channels and good stability. The porous FLPs behave unprecedented activity for atmospheric CO 2 activation and coupling with epoxides (25–40°C, 1 bar, without cocatalyst). This de novo assembly strategy exhibits good universality for synthesizing porous FLPs from different kinds of ILs, paving a facile approach for designing high-efficiency acidic–basic catalysts.
研究领域:
化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Zhige Zhang,Guofeng Zhao,Wenyang Li,Jiawei Zhong,Jun Xie
The efficient conversion of renewable biogas has attracted ever-increasing interest in past decades. Ni-CeO 2 -Al 2 O 3 supported on monolithic SiC-foam (denoted as Ni/CeO 2 -Al 2 O 3 /SCF) is designed and applied in biogas reforming. The monolithic Ni/CeO 2 -Al 2 O 3 /SCF catalysts were deeply characterized by XRD, ICP-AES, SEM, HR-TEM, CO 2 -TPD, etc. The cycle between CeO 2 -Al 2 O 3 and CeAlO 3 was verified by in-situ CH 4 /CO 2 -TPSR, and the catalytic role of CeAlO 3 in coke elimination and CO 2 activation was further confirmed. Due to the uniform distribution of Ni nanoparticles (NP S ) and the activation of CO 2 by CeAlO 3 , Ni/CeAlO 3 -Al 2 O 3 /SCF shows excellent catalytic stability to inhibit sintering and eliminate carbon deposition. At 900 °C and a gas hourly space velocity (GSHV) of 24000 mL g Cat -1 h −1 , excellent CH 4 /CO 2 conversion of 86/99% are initially achieved over Ni/CeAlO 3 -Al 2 O 3 /SCF catalyst, followed by slight decrease after 140 h, and remain basically stable for the next 260 h.
研究领域:
化学工程
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能源科学
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催化材料
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Ling Meng,Chenying Song,Qixuan Lin,Guanghang Sun,Jin Long,Xiting Zhang,Hailong Li,Jian Hu,Siyu Ye
Lithium–sulfur (Li–S) batteries have high theoretical energy density but low sulfur utilization due to the inherent insulating nature of sulfur and the shuttle effect of polysulfides. Herein, the CO2-activation carbon paper was prepared by poly(p-phenylenebenzobisoxazole) (PBO) nanofiber and was first applied as an interlayer for efficiently alleviating the shuttle effect of polysulfides in Li–S batteries. This interlayer exhibits good flexibility and strength with rich −C═O and −COOH functional groups on the three-dimensional porous structure, which improves chemical adsorption on Li2Sx species and ion rapid diffusion via interconnected diffusion channels and thus enhances the electrochemical kinetics. The initial specific capacity is 1367.4 mAh g–1 and remains 999.8 mAh g–1 after 200 cycles at 0.2C and 780.1 mAh g–1 at 5C, and the Coulombic efficiency is high, up to 99.8%, which is much better than that for the carbon paper without CO2 activation. The highly conductive flexible PBO carbon paper may bring breakthroughs in performance and thus lead to more practical applications of Li–S batteries.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）