FUEL
·
2024
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IF 6.7
Haiwen Xu,Danyang Li,Lei Jiang,Chunqiang Lu,Jiangyong Yuan,Zhiqiang Li,Yuelun Li,Huicong Zuo,Kongzhai Li
It is challenging to load precious metals nanoparticles on LaFeO 3 perovskite with small specific surface, and to improve the thermal stability of precious metals is also very difficult. Therefore, it is of great significance to disperse precious uniformly on perovskite with low specific surface area and to make the catalyst with high catalytic activity and thermal stability. In this work, we develop series of perovskite-based methane combustion catalysts with good catalytic activity and stability. Compare with traditional LaFeO 3 catalysts, the catalytic activity of three-dimensional ordered macroporous (3DOM) LaFeO 3 significantly improves by loading Pt. In addition, its thermal stability is significantly improved by adding CeO 2 , especially at high roasting temperature (800 °C). The 1 wt%Pt/10 %CeO 2 /3DOM LaFeO 3 catalysts shows the highest catalytic activity in which the T 10 , T 50 and T 90 are 362 °C, 433 °C and 502 °C, and its recaction temperature of T 50 is decreased by 50 °C compare with Pt/3DOM LaFeO 3 (8 0 0). The different physical and chemical characterizations suggest that the coupling of Ce 3+ and Fe 2+ induces the formation of a large number of oxygen vacancies, which promotes the oxygen mobility and th oxygen storage capacity during the methane oxidation process. More importantly, the CeO 2 addition contributes to the Pt-CeO 2 interaction with Ce-O-Pt bond formation, which greatly improves the thermal stability of the catalyst, and this Pt-CeO 2 interaction strength becomes more obvious with the increase of calcination temperature. Furthermore, the in-situ DRIFT experiments indicate that M−K mechanism is probably involved in the reaction process.
研究领域:
化学工程
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催化材料科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xuewu Deng,Xiaobing Zheng,Feifei Jia,Cuiyao Cao,Haolei Song,Yanjun Jiang,Yunting Liu,Guanhua Liu,Shijie Li,Lihui Wang
The selective oxyfunctionalization of C-H and C C bonds is highly important and catalyzed by unspecific peroxygenases (UPOs) which suffer from inactivation by hydrogen peroxide (H 2 O 2 ). Herein, photo-enzyme integrated catalysts were constructed by immobilizing Aae UPO as cross-linked enzyme aggregates (CLEAs) in Pd-loaded three-dimensional ordered macroporous titania (3DOM TiO 2 ) with in situ photocatalytic H 2 O 2 production. The prepared Aae UPO@3DOM TiO 2 -Pd obtained higher catalytic efficiency compared with CLEAs- Aae UPO. The conversion of ethylbenzene to (R) -1-phenethyl alcohol was significantly improved, reaching 99 % compared with free enzyme (38 %) and CLEAs- Aae UPO (49 %), with ee value of > 99 %. Aae UPO@3DOM TiO 2 -Pd exhibited good stability and reusability attributed to the protection of macropores and in situ H 2 O 2 production. By using the designed 3DOM platform for photocatalysis and enzyme immobilization, the in situ photocatalytic generation of H 2 O 2 was highly efficient, and the monodisperse CLEAs- Aae UPO in the macropores facilitated the contact of substrate and enzyme, thus obtaining excellent photo-enzyme coupled catalysis.
研究领域:
生物化学
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环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2023
·Vol. 34
·期 1
·1-12
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IF 2.8
Liang Xuan,Xue Suting,Wu Wangchen,Feng Qin,Zheng Xudong,Zhang Yakang,Xu Song,Zhou Man,Li Zhongyu
Herein, a series of CuS particles anchored three-dimensional ordered macroporous TiO 2 (CuS/3DOM-TiO 2 ) composites were fabricated by a biocompatible and environmental-friendly biomolecule-assisted route. For the first time in the macroporous 3DOM-TiO 2 , L-cysteine acted as multiple roles including sulfur source and chelating agent for anchoring of CuS particles. During the regulation by Cu/Ti molar ratios from 0.3 to 2, the average size of CuS particle which anchored on inner surface of 3DOM-TiO 2 was well-controlled from about 50 to 20 nm. The photocatalytic activities were investigated by visible-light degradation of methylene blue (MB). The highest activity of CuS/3DOM-TiO 2 was emerged when Cu/Ti equaled to 1. This optimized CuS/3DOM-TiO 2 -1 reached 99% in 180 min, which was 60% higher than that of pure TiO 2 . After four cycles, the photocatalytic activity of CuS/3DOM-TiO 2 retains more than 80% of its original performance. L-cysteine highly promoted the adhesion between CuS and TiO 2 which provided good cycling ability.
研究领域:
材料科学
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环境科学
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生物化学
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2021
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IF 7.92
Xiaohui Yu,Lingyun Dai,Jiguang Deng,Yuxi Liu,Lin Jing,Xing Zhang,Xiyun Jiang,Zhiquan Hou,Jia Wang,Hongxing Dai
SnO 2 is widely used in catalysis owing to its oxygen vacancies, reducible oxygen species, and acidity. In this work, Ru nanoparticles (NPs) supported on three-dimensionally ordered macroporous (3DOM) SnO 2 ( x Ru/3DOM SnO 2 , Ru loading ( x ) = 0.09–1.65 wt%) were fabricated via the polyvinyl alcohol-protected reduction routes, and their catalytic activities were determined for trichloroethylene (TCE) and/or toluene oxidation. It was shown that the 0.98Ru/3DOM SnO 2 sample exhibited the best activity and good thermal stability, with the temperature ( T 90% ) and apparent activation energy at a TCE (1000 ppmv) conversion of 90% being 300 °C and 44 kJ/mol at space velocity = 40,000 mL/(g h), respectively. Trichloromethane, carbon tetrachloride, tetrachloroethylene, and trichloroacetaldehyde hydrate were the main intermediates in TCE oxidation. The high catalytic performance of 0.98Ru/3DOM SnO 2 was attributed to the presence of hydroxyl groups adsorbed at the oxygen vacancies, strong O 2 adsorption ability, good low-temperature reducibility, and strong interaction between Ru NPs and 3DOM SnO 2 . In addition, a catalytic mechanism over x Ru/3DOM SnO 2 was proposed under dry and humid conditions. The introduction of H 2 O could block some of the reaction pathways from inhibiting the production of C 2 Cl 4 , reduce formation of some by-products (e.g., CH 2 Cl 2 , CH 3 COOH, and C 2 H 2 Cl 2 ), promote removal of the chlorine species, and generate a greater amount of HCl and a smaller amount of Cl 2 . Furthermore, introducing toluene into the TCE stream could generate smaller amounts of organic chlorine by-products and greater amounts of inorganic chlorine products (HCl and Cl 2 ). We are sure that this work can provide a guideline for the industrial application of supported Ru catalysts in the removal of Cl-containing volatile organic compounds.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
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2025
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IF 6.4
Ting-Ting Shen,Jing Liu,Fang-Yuan Bai,Wei-Wei Xu,Xue Yong,Zhi-Rong Li,Jing-Ru Han,Jun Chen,Heng Zhao,Zhi-Yi Hu,Yu Li,Bao-Lian Su
Biomass photoreforming to coproduce sustainable hydrogen and valuable chemicals is a potential strategy for alleviating energy and environmental issues. However, the lack of bifunctional catalysts to efficiently achieve the “one stone kills two birds” scenario greatly limits its practical application. Herein, we rationally design a three-dimensionally ordered macro-porous structure (3DOM) CaTiO3 (CTO) to address the mass diffusion and light harvesting and to load ZnxCd1-xS (ZxC1-xS) quantum dots (QDs) realizing the selective glucose photoreforming process. The regulatable band gap of ZxC1-xS endows 3DOM CTO-ZxC1-xS composites with sufficient light absorbance and adjustable redox potentials. As a result, the optimized 3DOM CTO-Z0.5C0.5S delivers the best performance for sustainable hydrogen evolution from glucose photoreforming with the rate of 4.05 mmol g-1 h-1 and the apparent quantum efficiency (AQY) of 6.48% under monochromatic light of 365 nm. In particular, the well-developed photocatalysts simultaneously produce gluconic acid with the selectivity up to 83.8% from the targeted oxidation of terminal aldehyde group of glucose. The DFT calculations on Gibbs free energy change of HER and the energy difference between reactants and products of OER further reveal that the constructed Z-scheme heterojunction contributes to the spatial separation of photogenerated electrons and holes for a good quantum efficiency and liquid product selectivity. This work demonstrates a sustainable technology for the coproduction of hydrogen and value-added chemicals from photocatalytic biomass valorization.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Guangjun Zhai,Jinguo Wang,Zimei Chen,Shuaifeng Yang,Yong Men
Three-dimensionally ordered macroporous (3DOM) Co 3 O 4 -CeO 2 catalysts with controllable Co/Ce molar ratios synthesized by colloidal crystal template method were developed to catalyze the NO x -assisted soot oxidation for the first time, and the obtained 3DOM Co 3 O 4 -CeO 2 catalysts exhibited highly enhanced soot oxidation activity. Detailed characterizations of 3DOM Co 3 O 4 -CeO 2 catalysts revealed that the highly enhanced soot oxidation activity was originated from the synergistic promoting effect by combining the macroporous effect resulted from the unique 3DOM framework, the chemical nature associated with more Co 3+ reactive sites, the surface enrichment of Ce species and the improved redox properties. Meanwhile, the high NO x storage and oxidation capacity resulted from the integrated respective merits of Co 3 O 4 and CeO 2 also accounted for the enhanced soot oxidation activity via NO x -assisted mechanism. Furthermore, the 3DOM Co 3 O 4 -CeO 2 catalysts demonstrated strong stability because of the surface enrichment of Ce species improving the thermal stability and the robust 3DOM framework inhibiting the structural collapse, showing their potential applications under practical conditions.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Dong Liu,Feiyang Hu,Yue Yan,Runping Ye,Xiaohan Chen,Bingying Han,Zhang-Hui Lu,Li Zhou,Gang Feng,Rongbin Zhang
CO oxidation is the primary approach for eliminating CO from incomplete combustion, and the catalytic performance is dependent on the structure of catalysts. Herein, to explore the structure promotion in the CO oxidation reaction, polymethyl methacrylate was synthesized as the hard template to fabricate the three-dimensional ordered microporous (3DOM) Au/CeO 2 and compared the catalytic performance with the Au/CeO 2 rod catalyst. The 3DOM Au/CeO 2 catalyst could realize complete CO oxidation at 90 °C while 110 °C for Au/CeO 2 rod catalyst. The 3DOM Au/CeO 2 catalyst also showed outstanding stability for 60 h reaction. The achieved high performance could be attributed to the pore structures and the better metal-support interaction that facilitates abundant oxygen vacancies . Additionally, the Au distribution and oxygen vacancies promoted by the macropores structures were discovered using a series of characterizations. This work highlights the promotion of oxygen vacancies and metal-support interaction by 3DOM structure in CO oxidation reaction.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Xueri Nan,Jing Liu,Xiuli Wang,Xianhui Pan,Xiaomei Wang,Xu Zhang
Three-dimensionally ordered macroporous cross-linked poly(glycidyl methacrylate) (3DOM) was constructed by water-soluble colloidal crystal templates and further functionalized with N-methyl-d-glucamine (NMDG) to prepare superhydrophilic adsorbents for boron removal from natural seawater. 3DOM adsorbents possess features of interconnected macropore structure, ultrathin pore wall, and superhydrophilicity, making efficient adsorption possible. The effect of cross-linking degree on the adsorption capacity toward boron was investigated. The NMDG-modified 3DOM adsorbent with rich vicinal diol functional groups showed superhydrophilicity and outstanding performance of adsorption. Significantly, its adsorption effect in boron removal from natural seawater indicated that the concentration of boron in natural seawater could decline to 0.16 from 4.24 mg·L–1 when the adsorbent dosage was 1 g·L–1, whereas the boron rejection reached 96.2%. After 10 regeneration–adsorption cycles, the adsorption capacity of 3DOM adsorbent remained over 85% of the initial value and the ordered structure was hardly changed. Additionally, 3DOM adsorbent could be directly and quickly separated from the seawater by a filter mesh of 16 mesh number. Research shows that the 3DOM adsorbent exhibits an adsorption performance for practical applications in boron removal from natural seawater.
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
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Desheng Yang,Chaofei Bai,Jiaran Liu,Shengnan Li,Chengzhao Tu,Fengdan Zhu,Guoping Li,Yunjun Luo,Tianfu Zhang
The construction of ordered pore structure and heterostructure interface is considered as an effective strategy to optimize the activity and stability of nano catalysts. Herein, we have elaborately fabricated the p-n heterostructure nanocatalysts of three-dimensionally ordered macroporous (3DOM) Fe 2 O 3 -supported 2D copper oxide nanofilm using a simple impregnation method, abbreviated as 3DOM-Fe 2 O 3 /CuO. The prepared 3DOM Fe 2 O 3 /CuO shows interconnected and ordered macroporous channels, which provide considerable catalytic active sites and enrich the reactive oxygen concentration at the Fe 2 O 3 -CuO heterostructure interface. By adjusting the copper source concentration, 2D copper oxide nanofilm with varied thicknesses was introduced to readily regulate the morphology of the catalyst and the atom composition or electronic structure of the interface. When evaluated as a catalyst for ammonium perchlorate (AP) decomposition reaction, 3DOM-Fe 2 O 3 /CuO-3 testified the most satisfactory catalytic activity, reducing the high temperature decomposition peak of AP decreased by 105.27 °C and the decomposition activation energy (Ea) by 50 %. Based on the experimental results of this study and related theoretical researches, the following mechanisms are proposed: in the thermal decomposition process of AP, the generation of active oxygen is not only related to the active oxygen mechanism, but also may be related to the NO 2 -assisted mechanism.
研究领域:
材料科学
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催化
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纳米技术
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2018
·
IF 4.667
Yue Chang,Ying Xuan,Chenxi Zhang,He Hao,Kai Yu,Shuangxi Liu
The core-shell shaped Pt@CdS nanoparticles were successful anchored onto the surface of three-dimensionally ordered macroporous (3DOM) SrTiO 3 with different pore sizes through a two-step photo-deposition method, to form a series of promising Z-scheme Pt@CdS/3DOM-SrTiO 3 composites for photocatalytic hydrogen evolution from water splitting. The well-ordered inverse opal and ternary heterojunction structure of Pt@CdS/3DOM-SrTiO 3 composites were well illustrated through SEM and HRTEM characterizations. The Pt@CdS/3DOM-SrTiO 3 composites exhibited excellent efficiency for hydrogen evolution (57.9 mmol/g h) under UV–vis light irradiation. Through a series of controlled experiments and related characterizations, the notably enhanced catalytic performance of Pt@CdS/3DOM-SrTiO 3 composites can be mainly attributed to the synergistic effect of the slow photon enhancement of 3DOM-SrTiO 3 , which significantly promotes the light harvesting efficiency of photocatalysts, and the enhanced separation of photogenerated carriers because of the Z-scheme charge transfer mechanism. In addition, the ternary Pt@CdS/3DOM-SrTiO 3 catalysts are very stable and can be recycled five times without any decrease in photocatalytic activity.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
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IF 4.3
Mengyun Lu,Xinwen Jia,Wenjing Zhang,Wuduo Zhao,Ajuan Yu,Gangfeng Ouyang
The enantioselective performance of porous chiral metal–organic frameworks (CMOFs) is closely related to the pore size and uniformity of easily accessible active sites. The chiral recognition efficiency of microporous CMOFs is hindered by the restricted diffusion of the guest. Hierarchical porous chiral CMOFs with multiple pore size regimes ranging from micropores to macropores have emerged as potential candidates in chiral separation applications. 3DOM Zn-MOF-74 crystalline porous material with ordered macro–micropore structure was prepared with a general bottom-up strategy by carrying out the controllable confined growth of Zn-MOF-74 precursor in a removable three-dimensional ordered macroporous (3DOM) polystyrene (PS) template. Then l-tryptophan ( l -Trp) was introduced into MOFs by the strategy of postsynthetic modifications, and finally, a chiral hierarchical porous functional material 3DOM Zn-MOF-74-l-Trp was successfully fabricated. Based on the two luminescent centers from the achiral ligand H4DOBC and chiral ligand l-Trp, the proportional fluorescence sensor 3DOM Zn-MOF-74-l-Trp was hopeful to be applied in the field of enantioselective fluorescence sensing. The enantioselectivity factor values of microporous M-Zn-MOF-74-l-Trp for 1,1′-bi-2-naphthol (Binol) and mandelic acid (MA) were 1.08 and 1.12, respectively. In comparison, the construction of hierarchical porous structure greatly enhanced the chiral recognition performance, which may be due to the improved mass-transfer efficiency of chiral guest molecules and highly swelled accessibility to the chiral recognition sites in this CMOF composite, making the enantioselectivity factor values correspondingly increased to 1.29 and 2.26, respectively.
研究领域:
材料科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysts
·
2023
·Vol. 14
·期 1
·18
·
IF 3.9
Kaixuan Chen,Linsheng Xu,Yuanfeng Li,Jing Xiong,Dawei Han,Yaxiao Ma,Peng Zhang,Haoqi Guo,Yuechang Wei
Herein, we present an in-depth investigation into the enhancement of catalytic soot oxidation through cerium-doped three-dimensional ordered macroporous (3DOM) La-Co-Ni-based perovskites synthesized with the colloidal crystal template (CCT) method. The 3DOM structure significantly contributes to the accessibility and interaction efficiency between soot and catalyst. Based on the results of powder X-ray diffraction (XRD), N2adsorption-desorption measurements, scanning electron microscopy (SEM), temperature-programmed oxidation of NO (NO-TPO), temperature-programmed reduction of H2(H2-TPR), in situ infrared Fourier transform spectroscopy (In-situ DRIFTS), and temperature-programmed oxidation (TPO) reactions, the role of cerium doping in modifying the structural and catalytic properties of 3DOM perovskite-type La2−xCexCoNiO6catalysts was investigated systematically. The optimized cerium doping ratio in La2−xCexCoNiO6catalysts can improve the microenvironment for efficient soot-catalyst contact, enhancing the catalytic activity of soot oxidation. Among the catalysts, the 3DOM La0.8Ce1.2CoNiO6catalyst shows the highest catalytic activity for soot oxidation, whose T10, T50, and T90values are 306 °C, 356 °C, and 402 °C, respectively. The mechanism of the cerium doping effect for boosting soot oxidation is proposed: The doping of Ce ions can increase the surface oxygen species, which is the main active species for promoting the key step of NO oxidation to NO2in catalyzing soot oxidation. This research provides a new strategy to develop high-efficient non-noble metal catalysts for soot oxidation in pollution control and sustainable environmental practices.
研究领域:
催化
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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
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