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Nanoconfinement effects of mesoporous CuMn2O4 spinel for constructing efficient Hg0 removal catalysts 用于构建高效除汞催化剂的介孔铜锰氧化物尖晶石的纳米细化效应
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106899
Yu Wang , Bin Zhou , Jingjie Guo , Tao Liu , Yu Yang , Bing Li , Jiaojiao Yang , Yue Peng , Jianjun Chen , Wenzhe Si , Junhua Li

Developing high-performance mercury removal catalysts is essential for addressing atmospheric mercury pollution. Notably, conventional mineral adsorbents are ineffective for high-temperature flue gases (>300 °C). In this study, confinement catalysis was utilized to modify CuMn2O4. Under the chlorine-free catalytic condition, the temperature window of T95 was widened by 150 °C (for 50–400 °C) toward high-temperature. Mechanistic studies suggest that nanoconfinement effects significantly improve the catalytic performance. Molecular oxygen adsorption and activation capacity were dramatically enhanced, as demonstrated by NAP-XPS. The plentiful grain boundaries effectively adjust the defect species and electronic structure of the catalysts in favor of Hg0 catalysis, whereas the porous structure improves the reactant adsorption properties.

开发高性能的脱汞催化剂对于解决大气汞污染问题至关重要。值得注意的是,传统的矿物吸附剂对高温烟气(>300 °C)无效。本研究利用封闭催化法对 CuMnO 进行了改性。在无氯催化条件下,T 的温度窗口向高温方向扩大了 150 °C(50-400 °C)。机理研究表明,纳米纤化效应显著提高了催化性能。NAP-XPS 证明,分子氧吸附和活化能力显著提高。丰富的晶界有效地调整了催化剂的缺陷种类和电子结构,有利于汞催化,而多孔结构则改善了反应物的吸附性能。
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引用次数: 0
Comprehensive investigation of solvent effects on BiOBr synthesis: Understanding the photocatalytic mechanisms of enrofloxacin and its degradation pathway 全面研究溶剂对 BiOBr 合成的影响:了解恩诺沙星的光催化机理及其降解途径
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106877
Yanli Sun , Xueliang Wang , Hooi Ling Lee

It is critical to enhance the photocatalytic performance of BiOBr through appropriate strategies. Two BiOBr samples with different water (W) and ethylene glycol (EG) solvents have been synthesized. BiOBr-EG presents a 3D nest-like morphology composed of nanoplates, prominently emphasizing (110) facets. In contrast, BiOBr-W displays 2D microplates with exposed (102) facets. Notably, BiOBr-EG exhibits a degradation rate 7.4 times faster and removal efficiency of Enrofloxacin (ENR) 2.2 times greater than that of BiOBr-W. Additional investigations reveal that ·O2 plays a dominant role in the degradation process. Finally, the degradation pathways are explored through DFT calculation and HPLC-MS methods.

通过适当的策略提高 BiOBr 的光催化性能至关重要。我们合成了两种以不同水(W)和乙二醇(EG)为溶剂的 BiOBr 样品。BiOBr-EG 呈现出由纳米板组成的三维巢状形貌,突出的是 (110) 面。相比之下,BiOBr-W 则呈现出二维微板,具有暴露的(102)面。值得注意的是,BiOBr-EG 的降解速度是 BiOBr-W 的 7.4 倍,恩诺沙星(ENR)的去除效率是 BiOBr-W 的 2.2 倍。其他研究表明,-O2- 在降解过程中起主导作用。最后,通过 DFT 计算和 HPLC-MS 方法探索了降解途径。
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引用次数: 0
Formic acid assisted synthesis of Cu-CuO-ZnO composite catalyst for acceptor free selective dehydrogenation of 1, 4-butanediol to γ-butrylactone 甲酸辅助合成 Cu-CuO-ZnO 复合催化剂,用于将 1,4-丁二醇无受体选择性脱氢为 γ-丁内酯
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106870
Paleti Gidyonu , Ajmeera Nagu , Sreedhar Gundekari , Mohan Varkolu

The Cu-CuO-ZnO composite catalyst synthesized through the formic acid-assisted method, underwent thorough characterization via XRD, N2 physisorption, TPR, TPD, TGA, XPS, and TEM. When applied to the selective dehydrogenation of 1,4-butanediol, this catalyst outperformed counterparts prepared through co-precipitation and impregnation methods. The superiority is attributed to the formic acid-assisted method yielding smaller Cu nanoparticles and some CuO species, undergoing in-situ reduction by dehydrogenation-generated H2. This process results in nascent Cu nanoparticles, enhancing catalytic performance. Notably, the catalyst demonstrated remarkable stability over a 100 h time-on-stream without discrepancies, highlighting the robustness of the formic acid-assisted method for 1,4-butanediol dehydrogenation.

通过甲酸辅助法合成的 Cu-CuO-ZnO 复合催化剂通过 XRD、N2 物理吸附、TPR、TPD、TGA、XPS 和 TEM 进行了全面表征。当应用于 1,4-丁二醇的选择性脱氢时,该催化剂的性能优于通过共沉淀和浸渍法制备的同类催化剂。其优越性归因于甲酸辅助法产生了较小的铜纳米颗粒和一些 CuO 物种,并通过脱氢产生的 H2 进行原位还原。这一过程会产生新的纳米铜颗粒,从而提高催化性能。值得注意的是,该催化剂在 100 小时的流化时间内表现出了显著的稳定性,没有出现任何偏差,这凸显了甲酸辅助法在 1,4-丁二醇脱氢过程中的稳健性。
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引用次数: 0
Catalytic ozonation of pharmaceutical compounds using carbon-based catalysts 使用碳基催化剂对药物化合物进行催化臭氧处理
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106863
C.A. Orge , C.A.L. Graça , J. Restivo , M.F.R. Pereira , O.S.G.P. Soares

Catalytic ozonation has become one of the most promising technologies for wastewater treatment due to its high efficiency in the removal of organic pollutants. Three carbon materials (carbon nanotubes, graphene oxide and activated carbon) and five pharmaceutical compounds were selected for this study. All tested parent pollutants were easily degraded by single ozonation. In terms of mineralization, the presence of catalyst revealed to be necessary to enhance organic matter removal, and activated carbon (GAC) showing superior performance. To evaluate the effect of the water matrix, experiments were performed with ground water and wastewater and significant degradation of pollutants was achieved.

催化臭氧技术在去除有机污染物方面具有很高的效率,因此已成为最有前途的废水处理技术之一。本研究选择了三种碳材料(碳纳米管、氧化石墨烯和活性炭)和五种药物化合物。所有测试的母体污染物都很容易被单一臭氧降解。在矿化方面,催化剂的存在对提高有机物去除率很有必要,而活性炭(GAC)则表现出更优越的性能。为了评估水基质的影响,使用地下水和废水进行了实验,结果表明污染物的降解效果显著。
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引用次数: 0
Synergistic catalytic performance of RuSn and PdCe composite catalysts for the hydrogenation of Terephthalic acid to 1,4-Cyclohexanedimethanol Ru Sn 和 Pd Ce 复合催化剂在对苯二甲酸加氢制 1,4-环己烷二甲醇过程中的协同催化性能
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106887
Ruijie Zhang, Haibo Jin, Lei Ma, Suohe Yang, Guangxiang He

1,4-cyclohexanedimethanol (CHDM) is used as a high-value polyester monomer. On the basis of the catalysts of RuSn and Pd, the compound catalysts of RuSn and PdCe are prepared by adding the additive Ce to the Pd-based catalyst. The results showed that the yield of CHDM increased by 13.4% after the addition of Ce, indicating that Ce is conducive to the activation of HH and CO thus promoting the hydrogenation of carboxyl groups. Furthermore, the addition of Ce effectively slows down the coverage of the compound on the active component Pd, prolonging the lifespan of the catalyst.

1,4-Cyclohexanedimethanol (CHDM) 是一种高价值的聚酯单体。在 RuSn 和 Pd 催化剂的基础上,通过在 Pd 基催化剂中添加添加剂 Ce,制备了 RuSn 和 PdCe 复合催化剂。结果表明,添加 Ce 后,CHDM 的产率提高了 13.4%,这表明 Ce 有利于活化 HH 和 CO,从而促进羧基的氢化。此外,Ce 的添加还有效减缓了化合物对活性成分钯的覆盖,延长了催化剂的使用寿命。
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引用次数: 0
Preparation of CuO-Bi2O3/SiO2@TiO2 core-shell structured catalysts and its catalytic performance for synthesis of 1, 4-butynediol by ethynylation of formaldehyde CuO-Bi2O3/SiO2@TiO2 核壳结构催化剂的制备及其在甲醛乙炔化合成 1,4-丁炔二醇中的催化性能
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106889
Gang Guan , FengYun Ma , Ping Luo , XiaoLin Zhang , XiaoDing Li , GuangXing Li

CuO-Bi2O3/SiO2@TiO2 core-shell structured catalysts were prepared by stepwise precipitation method and used for the synthesis of 1, 4-butynediol (BYD) by the ethynylation of formaldehyde. The characterization results, by XRD, BET, SEM, TEM, TPD etc., revealed the TiO2 content not only affecting the surface area of the catalysts and the partical size of the loaded CuO, but also affecting the electronic interactions with CuO. The activity tests showed that the catalyst with 20% TiO2 calcined at 450 °C had a short activation time, with good activity with conversion 91% and BYD yield 73% after 6 h on line. The catalysts still maintained good catalytic activity and stability after 6 repeated uses. ICP data indicate that leaching of Cu active component after reaction is very low.

采用分步沉淀法制备了 CuO-BiO/SiO@TiO 核壳结构催化剂,并将其用于甲醛乙炔化反应合成 1,4-丁炔二醇(BYD)。XRD、BET、SEM、TEM、TPD 等表征结果表明,TiO 含量不仅会影响催化剂的表面积和负载 CuO 的粒径,还会影响与 CuO 的电子相互作用。活性测试表明,含 20% TiO 的催化剂在 450 °C 煅烧时活化时间短,活性好,上线 6 小时后转化率达 91%,比亚迪收率达 73%。重复使用 6 次后,催化剂仍保持良好的催化活性和稳定性。ICP 数据表明,反应后 Cu 活性组分的浸出率非常低。
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引用次数: 0
Synergistic enhancement of visible light Photocatalysis: Tailoring dual Z-scheme Fe2O3/C3N4/NH2-MIL-125 ternary composites for organic pollutant degradation 可见光光催化的协同增强:定制用于有机污染物降解的双 Z 型 Fe2O3/C3N4/NH2-MIL-125 三元复合材料
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106893
Li-Heng Kao , Jun-Jie Liu , To-Yu Wang , Duo-Syuan Lin , Ying-Shuo Cheng , Chia-Hao Tseng , Kanit Manatura , Wei-Yu Chen , Kun-Yi Andrew Lin , Chao-Wei Huang

In this study, Fe2O3/C3N4/NH2-MIL-125 ternary composite photocatalysts were synthesized. Their amino groups provided close bonding between these materials, facilitating the effective separation of electrons and holes. Besides, each component of Fe2O3/C3N4/NH2-MIL-125 plays a crucial role. NH2-MIL-125 provided a high surface area, C3N4 contributed to the primary photocatalytic activity, and Fe2O3 aided in enhancing light absorption, generating additional potential to produce hydroxyl radicals, thereby further enhancing photocatalytic activity. Moreover, the proportion of loaded Fe2O3 and C3N4 in the ternary material was investigated. It was found that Fe2O3/C3N4/NH2-MIL-125 with a 1:1 ratio of Fe2O3 and C3N4 (FeCN1:1/NM125) exhibited excellent photocatalytic performance, in which RhB degradation reached 100% under visible light irradiation, conforming to first-order kinetics analysis with a reaction rate constant k of 0.0164 min−1. Its efficiency was twice that of the binary catalyst C3N4/NH2-MIL-125 or Fe2O3/NH2-MIL-125, seven times that of the pristine catalyst C3N4, and ten times that of the pristine catalyst NH2-MIL-125. Scavenger experiments showed that the degradation efficiencies were 52.57%, 55.51%, and 63.41%, respectively, indicating that three active species, namely superoxide radicals, holes, and hydroxyl radicals, made significant contributions to photocatalysis.

本研究合成了 FeO/CN/NH-MIL-125 三元复合光催化剂。FeO/CN/NH-MIL-125是一种三元复合光催化剂,其氨基酸基团使这些材料之间紧密结合,从而促进了电子和空穴的有效分离。此外,FeO/CN/NH-MIL-125 中的每种成分都起着至关重要的作用。NH-MIL-125 提供了高比表面积,CN 促进了主要的光催化活性,而 FeO 则有助于增强光吸收,产生更多的羟基自由基,从而进一步提高光催化活性。此外,还研究了三元材料中负载的 FeO 和 CN 的比例。研究发现,FeO/CN/NH-MIL-125 中 FeO 和 CN 的比例为 1:1(FeCN1:1/NM125),具有优异的光催化性能,在可见光照射下,RhB 降解率达到 100%,符合一阶动力学分析,反应速率常数 k 为 0.0164 分钟。其效率是二元催化剂 CN/NH-MIL-125 或 FeO/NH-MIL-125 的两倍,原始催化剂 CN 的七倍,原始催化剂 NH-MIL-125 的十倍。清除剂实验表明,降解效率分别为 52.57%、55.51% 和 63.41%,这表明超氧自由基、空穴和羟基自由基这三种活性物种在光催化中做出了重要贡献。
{"title":"Synergistic enhancement of visible light Photocatalysis: Tailoring dual Z-scheme Fe2O3/C3N4/NH2-MIL-125 ternary composites for organic pollutant degradation","authors":"Li-Heng Kao ,&nbsp;Jun-Jie Liu ,&nbsp;To-Yu Wang ,&nbsp;Duo-Syuan Lin ,&nbsp;Ying-Shuo Cheng ,&nbsp;Chia-Hao Tseng ,&nbsp;Kanit Manatura ,&nbsp;Wei-Yu Chen ,&nbsp;Kun-Yi Andrew Lin ,&nbsp;Chao-Wei Huang","doi":"10.1016/j.catcom.2024.106893","DOIUrl":"10.1016/j.catcom.2024.106893","url":null,"abstract":"<div><p>In this study, Fe<sub>2</sub>O<sub>3</sub>/C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 ternary composite photocatalysts were synthesized. Their amino groups provided close bonding between these materials, facilitating the effective separation of electrons and holes. Besides, each component of Fe<sub>2</sub>O<sub>3</sub>/C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 plays a crucial role. NH<sub>2</sub>-MIL-125 provided a high surface area, C<sub>3</sub>N<sub>4</sub> contributed to the primary photocatalytic activity, and Fe<sub>2</sub>O<sub>3</sub> aided in enhancing light absorption, generating additional potential to produce hydroxyl radicals, thereby further enhancing photocatalytic activity. Moreover, the proportion of loaded Fe<sub>2</sub>O<sub>3</sub> and C<sub>3</sub>N<sub>4</sub> in the ternary material was investigated. It was found that Fe<sub>2</sub>O<sub>3</sub>/C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 with a 1:1 ratio of Fe<sub>2</sub>O<sub>3</sub> and C<sub>3</sub>N<sub>4</sub> (FeCN1:1/NM125) exhibited excellent photocatalytic performance, in which RhB degradation reached 100% under visible light irradiation, conforming to first-order kinetics analysis with a reaction rate constant k of 0.0164 min<sup>−1</sup>. Its efficiency was twice that of the binary catalyst C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 or Fe<sub>2</sub>O<sub>3</sub>/NH<sub>2</sub>-MIL-125, seven times that of the pristine catalyst C<sub>3</sub>N<sub>4</sub>, and ten times that of the pristine catalyst NH<sub>2</sub>-MIL-125. Scavenger experiments showed that the degradation efficiencies were 52.57%, 55.51%, and 63.41%, respectively, indicating that three active species, namely superoxide radicals, holes, and hydroxyl radicals, made significant contributions to photocatalysis.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106893"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000530/pdfft?md5=88a7045d6c20ae52271cd0fd7a71553a&pid=1-s2.0-S1566736724000530-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140054649","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Improving catalytic activity of MoP for CO2 reforming of methane via ZrO2 modification 通过 ZrO2 改性提高 MoP 在 CO2 甲烷转化中的催化活性
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106902
Yan Kong , Long Tian , Guiming Xie , Xiaorui Wang , Yi Man , Zhou-jun Wang

Molybdenum phosphide (MoP) has attracted increasing attention as a novel catalytic material for CO2 reforming of methane in virtue of superior coke resistance, but its catalytic reactivity is still relatively low. This work for the first time improved the reforming activity of MoP via ZrO2 modification. The Zr0.01MoP catalyst with Zr/Mo molar ratio of 0.01 possessed much higher activity than bare MoP at 800–900 °C. Structural characterizations revealed that the introduction of ZrO2 would decrease the particle size, modify the electronic structure and change the reducibility property of MoP, which may function together to deliver the higher activity.

磷化钼(MoP)作为一种新型甲烷一氧化碳重整催化材料,以其优异的抗焦化性而受到越来越多的关注,但其催化反应活性仍然相对较低。这项研究首次通过氧化锆改性提高了 MoP 的重整活性。Zr/Mo 摩尔比为 0.01 的 ZrMoP 催化剂在 800-900 ℃ 下的活性远高于裸 MoP。结构表征显示,氧化锆的引入会减小 MoP 的粒度、改变其电子结构并改变其还原性,这些因素可能共同作用提高了活性。
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引用次数: 0
Magnetically retractable tea extract stabilized palladium nanoparticles for denitrogenative cross-coupling of aryl bromides with arylhydrazines under green conditions: An alternate route for the biaryls synthesis 磁性可伸缩茶叶提取物稳定钯纳米粒子在绿色条件下用于芳基溴与芳基肼的变性交叉偶联:双芳基合成的另一条途径
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106862
Sumanth Hegde, Aatika Nizam

Novel palladium based magnetic nanocatalyst was synthesized by the co-precipitation method and coated with silica and tea extract as stabilizing agent. Palladation onto the prepared nanocomposite was done to get ION-SiO2/TE-Pd(0) catalyst. Our study is one of the limited number of studies reported for the catalytic denitrogenative coupling of arylbromide and arylhydrazine. This led to the construction of important substituted biaryls bearing various substituents with 82–92% yields. The synthesized nanocatalyst was characterized using structural and morphological characterization techniques. It was also observed that only 2 mol% of ION-SiO2/TE-Pd(0) catalyst was sufficient for the catalysis and reusable upto six cycles.

采用共沉淀法合成了新型钯基磁性纳米催化剂,并以二氧化硅和茶叶提取物作为稳定剂进行了包覆。在制备的纳米复合材料上进行钯化,得到 ION-SiO2/TE-Pd(0) 催化剂。我们的研究是关于芳基溴和芳基肼催化脱氮偶联的少数研究之一。通过这项研究,我们以 82-92% 的收率合成了含有各种取代基的重要取代双芳基化合物。利用结构和形态表征技术对合成的纳米催化剂进行了表征。研究还发现,仅 2 摩尔%的 ION-SiO2/TE-Pd(0) 催化剂就足以进行催化,并且可重复使用长达六个循环。
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引用次数: 0
Tailoring Cu immobilized MCM-41-based mesostructured catalysts for selective hydrogenolysis of biomass-derived furfural 定制铜固定化 MCM-41 介质结构催化剂,用于生物质衍生糠醛的选择性氢分解
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106898
Leela Prasad Yandrati , Swamy Sekhar Kaladi , Raveendra Gundeboyina , Ramakrishna Pothu , Vijaya Moli , B. Venkateswara Rao , Rajender Boddula Ph.D. , Rammohanrao Devulapalli , Harisekhar Mitta Ph.D.

The CuO-supported MCM-41 catalysts were prepared using a simple incipient wet impregnation method. The catalysts were investigated for hydrogenation of furfural to furfuryl alcohol synthesis. Among all the catalysts, the 2.5% CuO/MCM-41 catalyst shows the best catalytic performance with 92.5% conversion and 89% selectivity of furfuryl alcohol at 210 °C. The catalyst also demonstrated a high turnover frequency (TOF) of 154.4 h−1. The 2.5% CuO/MCM-41 catalyst remained stable for up to 20 h during the time on stream.

采用简单的惰性湿浸渍法制备了 CuO 支持的 MCM-41 催化剂。研究了催化剂在糠醛加氢合成糠醇中的应用。在所有催化剂中,2.5% CuO/MCM-41 催化剂的催化性能最好,在 210 ℃ 时,糠醇的转化率为 92.5%,选择性为 89%。该催化剂还显示出 154.4 h-1 的高翻转频率 (TOF)。2.5% CuO/MCM-41 催化剂在长达 20 小时的流动过程中保持稳定。
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引用次数: 0
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Catalysis Communications
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