Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 4
·1-15
·
IF 4.3
Guo Yunyu,Wang Yiran,Shao Yuewen,Zhang Shu,Wang Yi,Hu Song,Xiang Jun,Hu Xun
During steam reforming, the performance of a catalyst and amount/property of coke are closely related to reaction intermediates reaching surface of a catalyst. Herein, modification of reaction intermediates by placing Mg-Al-hydrotalcite above Ni/KIT-6 catalyst in steam reforming of glycerol was conducted at 300 to 600 °C. The results revealed that the catalytic activity of Ni/KIT-6 in the lower bed was enhanced with either Mg 1 -Al 5 -hydrotalcite (containing more acidic sites) or Mg 5 -Al 1 -hydrotalcite (containing more alkaline sites) as upper-layer catalyst. The in situ infrared characterization of steam reforming demonstrated that Mg-Al-hydrotalcite catalyzed the deoxygenation of glycerol, facilitating the reforming of the partially deoxygenated intermediates over Ni/KIT-6. Mg-Al-hydrotalcite as protective catalyst, however, did not protect the Ni/KIT-6 from formation of more coke. Nonetheless, this did not lead to further deactivation of Ni/KIT-6 while Mg 5 -Al 1 -hydrotalcite even substantially enhanced the catalytic stability, even though the coke was much more significant than that in the use of single Ni/KIT-6 (52.7% vs. 28.6%). The reason beneath this was change of the property of coke from more aliphatic to more aromatic. Mg 5 -Al 1 -hydrotalcite catalyzed dehydration of glycerol, producing dominantly reaction intermediates bearing C=C, which formed the catalytic coke of with carbon nanotube as the main form with smooth outer walls as well as higher aromaticity, C/H ratio, crystallinity, crystal carbon size, thermal stability, and resistivity toward oxidation on Ni/KIT-6 in the lower bed. In comparison, the abundance of acidic sites on Mg 1 -Al 5 -hydrotalcite catalyzed the formation of more oxygen-containing species, leading to the formation of carbon nanotubes of rough surface on Ni/KIT-6.
研究领域:
催化
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化学工程
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材料科学
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能量转换
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表面化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shiying Fan,Yao Liu,Zetao Zhang,Mengnan Huang,Yuejiao Wang,Jing Gao,Ying Xiong
Three-dimensional mesoporous silica is a distinctive nanomaterial celebrated for its unique structure, substantial specific surface area, enhanced utilization of active surfaces, and improved adsorption and catalytic reaction capabilities. Nevertheless, its limited surface functional groups often impede its effective ion adsorption capacity. Here, inspired by the mussel-adhesive phenomenon, in this study, we introduced a straightforward layer-by-layer assembly approach to fabricate a new series of KIT-6@x-catechol/polyethyleneimine composites, the catechol/polyethyleneimine is the shell and KIT-6 is the core. Importantly, catechol(CA) and polyethyleneimine(PEI) polymers as selective layers with dense structures and abundant cation exchange groups, resulting in outstanding adsorption performance for our material. At a pH of 3.0, Ga(III) exhibited a maximum adsorption capacity of 88.65 mg g −1 on the adsorbent. Furthermore, the adsorbent demonstrated selective adsorption capabilities for Ga(III) over Ge(IV), Al(III), Cu(II), Zn(II), and Co(II). The primary adsorption mechanism of KIT-6@x-CA/PEI is chelation that occurs through coordination between the O atom on the phenolic hydroxyl group of CA and Ga 3+ , Ga(OH) 2+ , Ga(OH) 2 + under pH 3.0 conditions. In summary, the synthesized KIT-6@x-CA/PEI exhibits significant potential for water treatment containing Ga(III) through adsorption processes.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhengang Zhou,Junjie Zheng,Lingyu Shao,Xiao Zhang,Chengjin Pan,Xiuqi Hu,Kai Feng,Hao Song,Shihan Zhang,Chenghang Zheng,Xiang Gao
Catalytic solvent regeneration has garnered significant attention due to its capacity to lower energy demands in industrial processes, promoting broader adoption of carbon capture systems. While progress has been made in catalyst engineering, creating efficient solid acid catalysts still encounters critical obstacles such as synthesizing mesoporous architectures with extensive surface areas and improving the spatial arrangement of active sites. Herein, this study developed a Ni/Fe@KIT-6 catalyst with ordered porosity and dual metal acid sites, leveraging the three-dimensional cubic pore structure of mesoporous silica to enhance liquid-solid mass transfer. The anchored Ni/Fe clusters synergistically enhanced proton transfer, reducing the activation energy of carbamate decomposition through optimized intermediate adsorption configurations. Catalytic testing revealed a 58.1 % enhancement in CO₂ desorption efficiency alongside a 41.2 % decrease in energy requirements relative to non-catalytic systems. The material maintained stable performance across multiple absorption-desorption cycles (efficiency decline <10 %), linked to the KIT-6 framework's retained structural stability and optimized metal-support bonding. Theoretical calculations revealed that the Ni/Fe dual sites lowered the CO 2 desorption reaction energy barrier, aligning with the enhanced CO₂ desorption efficiency. This synergistic interaction of dual metal acid sites within a high-surface-area architecture highlights viable pathways for scalable and energy-efficient CO₂ desorption, thereby advancing practical strategies for large-scale deployment of carbon capture technologies.
研究领域:
催化化学
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碳捕集与封存
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材料科学
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化学工程
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环境科学
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产品关联
DOI
高影响因子
ENERGY & FUELS
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2020
·
IF 3.421
Peijing Shao,Han Chen,Qin Ying,Shihan Zhang
In order to fulfill the application of carbonic anhydrase (CA) in the carbon dioxide capture process, immobilization technology will be used to enhance the stability of the enzyme. The structure of the support for the enzyme immobilization is important to determine the enzyme activity and stability. In this work, mesoporous molecular sieves with different dimensions and pore sizes were used as supports for the immobilization of CA. Characterization analysis indicated that the carrier material retained its integrity after enzyme immobilization. The half-life (t1/2) of CA/KIT-6, CA/SBA-15, and CA/MCM-41 increased to 3.0, 2.8, and 2.0 times compared to the free CA enzyme. Additionally, the experimental results showed that when using SBA-15 with a two-dimensional structure and a large pore size as the carrier, the CA enzyme loading was high and retained 78% relative activity and 98% initial activity after 6 days at 40 °C. Comprehensively, CA/SBA-15 was more suitable for capturing CO2 in flue gas than CA/MCM-41 and CA/KIT-6.
研究领域:
生物化学
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环境科学
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产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2018
·
IF 3.849
He Yang,Weiqi Wei,Shubin Wu,Junping Zhuang
During the upgrading into biorefinery factories, the traditional pulp and paper mills urgently need to broaden the applications of pulp to achieve higher economic benefits. The conversion of pulp into high value-added bulk chemicals is considered as a potential approach. The pulp was previously treated by HCl and spray drying to decrease its particle size to 71.4 μm as the catalytic raw material. Mesoporous WO 3 with the specific surface area of 58.6 m 2 /g was then synthesized via KIT-6 silica template and it shown high performance in catalytic conversion of pretreated pulp into ethylene glycol. The feedstock conversion was 100% and the yield of ethylene glycol was 62.7% under the optimum condition. In comparison tests, the pretreated pulp and mesoporous WO 3 both displayed better catalytic performance than untreated pulp and nano-sized WO 3 without porous structure. However, the catalytic performance of mesoporous WO 3 decreased in recycling test and the reasons were analyzed preliminarily. This work demonstrated that the ordered mesoporous WO 3 was a high-performance catalyst and had potential for producing ethylene glycol in good cooperation with acid pretreated pulp.
研究领域:
化学工程
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生物质转化
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催化材料
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产品关联
DOI
高影响因子
ACS Omega
·
2019
·
IF 2.584
Chengxiang Shi,Huan Wang,Qiulin Bi,Liqing Li,Pingchuan Sun,Tiehong Chen
Hierarchically porous silica KIT-6 and SBA-15 mesostructures were successfully synthesized by using a mesomorphous complex of a nonionic triblock copolymer (pluronic P123) and an anionic polyelectrolyte (polyacrylic acid) as the dynamic template. The obtained mesoporous silica materials possessed both ordered mesopores (∼7 nm) and nanopores (∼15–50 nm), and the long-range order of the mesophase was not perturbed by the embedded larger secondary nanopores. Moreover, hierarchically porous silica KIT-6 exhibited enhanced adsorption capacity in enzyme and protein immobilization, which was attributed to the hierarchically porous structure.
研究领域:
材料科学
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生物技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2026
·
IF 3.4
Jiaying Liu,Shiwei Wang,Dong Wang,Zhihao Yu,Lin Zhu,Chunzheng Wu,Hongbo Yu
Modifying noble metal catalysts with transition metal oxides (MOx) is an effective strategy to enhance both catalytic activity and selectivity through interfacial synergy. However, achieving precise spatial colocalization of the metal and oxide phases remains a challenge. Herein, Pd1-(CuOx)1 hybrid nanostructures confined within KIT-6 mesoporous silica were rationally synthesized via in situ oxidative transformation of PdCu bimetallic nanoparticles (NPs) under controlled thermal treatment. The resulting Pd1-(CuOx)1/KIT-6 catalysts exhibited markedly enhanced activity and chemoselectivity for the hydrogenation of acetophenone to 1-phenylethanol compared with monometallic Pd/KIT-6 and PdCu/KIT-6. The optimal catalyst with a Pd/Cu molar ratio of 1:1 achieved 93.1% acetophenone conversion and 98.2% selectivity toward 1-phenylethanol, and demonstrated broad applicability across a range of ketone substrates. Comprehensive structural characterization revealed that the Pd-CuOx interfacial sites are central to the observed performance enhancement: metallic Pd facilitates H2 dissociation, while adjacent CuOx species are proposed to facilitate carbonyl adsorption, contributing to the overall synergistic enhancement. This interface-driven synergistic mechanism provides a general, efficient, and cost-effective strategy for the selective hydrogenation of multifunctional molecules.
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DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2023
·
IF 3.4
Lihong Guo,Wenlei Xie,Xiangxin Xu
BACKGROUND The exploration of a robust solid acid catalyst for the efficient hydrolysis of cellulose is a research hotspot due to the need for clean production and sustainable development. KIT-6 silica offers abundant three-dimensionally interconnected mesopores, which are expected to be superior to mesoporous structures with one- or two-dimensional channels due to faster diffusion of reactants and products during reaction. The catalytic conversion of microcrystalline cellulose is examined in detail over a functionalized KIT-6 catalyst prepared by the method of Zr addition and subsequent sulfation. RESULTS In terms of cellulose conversion and product yield, the activity of the catalysts followed the order of sulfated Zr-KIT-6 > Zr-KIT-6 > SO 4 2− -KIT-6 > KIT-6. Over the sulfated Zr-KIT-6 catalyst with a Si/Zr molar ratio of 7:1, a maximum cellulose conversion of 95.0% was achieved with glucose yield of 23.4%, 5-hydroxymethylfufural yield of 4.9% and levulinic acid yield of 11.7% under the optimized reaction conditions: reaction temperature of 200 °C, reaction time of 2 h, catalyst amount of 0.3 g, cellulose-to-water mass ratio of 1:1. CONCLUSION The sulfated Zr-KIT-6 catalyst possessed the strongest and richest Brønsted acid sites, which readily provided protons for the cleavage of β -1,4 glycosidic bonds in cellulose, thus conferring superior catalytic activity in cellulose hydrolysis. A plausible pathway at the initial stage of cellulose hydrolysis over the catalyst was proposed. © 2023 Society of Chemical Industry (SCI).
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2025
·
IF 4.2
Yifan Zhang,Jiaying Liu,Shiwei Wang,Zhihao Yu,Haojian Zhang,Dong Wang,Lin Zhu,Chunzheng Wu,Hongbo Yu
Modifying noble metal catalysts with transition metal oxides (MO x ) can markedly enhance catalytic performance through synergistic effects, yet precise spatial colocalization of active metal and promoter phases remains challenging. Here, we report the synthesis of KIT-6 supported Pd-MO x (M = Fe, Co, Ni) hybrid nanostructures via in situ transformation of bimetallic PdM nanoparticles under controlled thermal conditions. The resulting Pd-MO x /KIT-6 catalysts displayed superior activity and selectivity in the selective hydrogenation of acetophenone to 1-phenylethanol compared with monometallic Pd/KIT-6. Among them, Pd-CoO x /KIT-6 (Pd/Co=1:1) achieved the highest performance, with 99.7% acetophenone conversion and 98.2% selectivity, and demonstrated broad applicability for hydrogenating diverse ketones. Structural and kinetic studies revealed that interfacial Pd-CoO x sites play a pivotal role: Pd domains efficiently dissociate H 2 , while CoO x species enhance acetophenone adsorption. This synergistic interface-driven mechanism provides a general and costeffective strategy for the selective hydrogenation of multifunctional substrates.
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产品关联
DOI
高影响因子
ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY
·
2014
·Vol. 20
·期 7
·883-888
·
IF 1.735
Zhang Zhongzheng,Wang Hui,Chen Xinqing,Xie Rongyong,Gao Peng,Wei Wei,Sun Yuhan
The sorption isotherms of CO 2 in wet ordered mesoporous silica KIT-6 with different amounts of pre-adsorbed water were firstly collected experimentally using a volumetric method in the temperature range of 275–281 K. The isotherms show an inflection point indicating CO 2 hydrates form in the pore spaces which is proofed by the enthalpy change calculated at the inflection pressure, and the quantity of water content shows considerable effect on the sorption capacity of CO 2 . The highest enhancement of sorption capacity in the presence of water is observed in wet KIT-6 sample with water loadings of 2.48, which is about 12.80 mmol/g and 1.86 times than that on dry sample. However, the saturation capacity is still far less than that what can be stored merely in the form of hydrates due to the low ratio of water utilization because of the large pore and the polar surface of KIT-6.
研究领域:
材料科学
·
环境工程
·
吸附技术
·
碳捕集与封存
✓ 已验证
DOI
高影响因子
RENEWABLE ENERGY
·
2023
·
IF 8.7
Qiaofei Zhang,Wenlei Xie,Jiangbo Li,Lihong Guo
For the purpose of fabricating an efficient solid acid catalyst for biodiesel production from low-grade acidic oils, bimetallic silica mesoporous composites with different Zr/Al molar ratios were initially synthesized via a facile one-step hydrothermal method , and then sulfated with sulfuric acid at different concentrations to get a series of sulfated Zr x -Al y -KIT-6 catalysts (denoted as SZA-K, where x/y represents the molar ratio of Zr to Al). The sulfated bimetallic solid catalysts were fully characterized by using XRD , FT-IR, TEM, SEM, EDS, NH 3 -TPD, and nitrogen porosimetry measurements. Results showed that the remarkable amount of acidic sites in the catalysts was derived from the Zr and Al incorporation and further sulfation, and specifically, the Zr 4+ and Al 3+ could afford abundant weak acid sites while the inductive effect of SO 4 2− species greatly influences the acidic strength of this solid catalyst. In combination with the enhancement in mass transfer resulting from the inherent interconnected mesoporous structure, the SZA-K catalyst could facilitate the transesterification reaction to take place efficiently. The sulfated Zr 5 –Al 1 -KIT-6 catalyst (Zr/Al molar ratio of 5/1, treated using 0.75 mol/L sulfuric acid for 12 h) exhibited enhanced acid strength with larger number of acidic sites (7.81 mmol/g), resulting in a high catalytic performance to the oil transesterification reaction. An oil conversion of 96.3% was attained for the transesterification reaction performed at 120 °C for 7 h by using a methanol/oil molar ratio of 20:1 and a catalyst dosage of 6 wt%. Further, this solid catalyst exhibited better acid and water-resistance capacity with above 80% of oil conversion even with 10% of free fatty acid (FFA) and 2% of moisture present in the low-grade acidic oils. Meanwhile, the good reusability was shown for this catalyst with 80.1% conversion even after reusing for three cycles. The good stability of the solid catalyst was resulted from the strong interactions between the acidic species and the bimetallic composite support.
研究领域:
化学工程
·
催化材料
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2013
·
IF 4.814
Bin Hu,Huan Liu,Kai Tao,Chunrong Xiong,Shenghu Zhou
Tungsten-doped mesoporous KIT-6 (W-KIT-6), mesoporous silica supported WO3/KIT-6, and traditional silica supported WO3/SiO2 catalysts have been successfully synthesized and tested for catalytic metathesis of 1-butene and ethene to propene. The resultant materials were comprehensively characterized by XRD, BET, TEM, UV–DRS, IR, XPS, H2-TPR, and TGA. For W-KIT-6 catalysts, high concentration of W5+ species by XPS and the difficulty of reduction of W species by TPR suggested the incorporation of W species into the KIT-6 framework. The studies of small-angle XRD, BET, and TEM illustrated that the 3D ordered mesoporous structure and their high surface area of KIT-6 were maintained in W-KIT-6. The doped W-KIT-6 illustrated superior catalytic performance to the supported WO3/KIT-6 and WO3/SiO2 catalysts. The origin of catalytic performance enhancement for W-KIT-6 was preliminarily discussed and was assigned to the incorporation of W species into KIT-6 framework. This study demonstrated the influence of neighboring environment of active components on catalytic performance and was helpful to design metathesis catalysts.
研究领域:
催化化学
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材料科学
·
化学工程
·
无机化学
·
多孔材料
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）