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Nickel and Molybdenum-Containing Perovskites as Efficient Heterogeneous Catalysts for the Conversion of Biobased Furfural to a Fuel Additive Intermediate 含镍和钼的包闪石作为高效异相催化剂将生物基糠醛转化为燃料添加剂中间体
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1007/s10562-024-04864-y
Ketshepile Baabua, Phadishe S. Pole, Ndzondelelo Bingwa

In this work, the catalytic conversion of furfural was found to follow both CTHs and etherification pathways in one-pot over multicationic inorganic perovskites (LaNi1-xMoxO3±δ) as heterogeneous catalysts. The conversion of furfural (FA) into alcohols and ether functionalities using the as-synthesized perovskite catalysts showed good conversions that are above 80% and excellent selectivity towards the desired product. The LaMoO3 catalyst was found to achieve the highest percentage conversion of 83%. Simple and multicationic inorganic perovskites were successfully employed in the transformation of furfural to produce β-methoxy-2-furanethanol. Furthermore, we postulate the hydrogenation of the keto-group to be the first step in the mechanism of the formation of β-methoxy-2-furanethanol and that its formation is characterized by rearrangement of the intermediate over the surface of the catalyst.

Graphical abstract

在这项工作中,发现在多元无机过氧化物(LaNi1-xMoxO3±δ)作为异相催化剂上,糠醛的催化转化遵循一锅双酚和醚化途径。使用合成的过氧化物催化剂将糠醛(FA)转化为醇和醚官能团的过程显示出良好的转化率,超过 80%,并且对所需产物具有极佳的选择性。LaMoO3 催化剂的转化率最高,达到 83%。在糠醛转化生成 β-甲氧基-2-呋喃乙醇的过程中,我们成功地使用了简单和多元无机包晶石。此外,我们推测酮基的氢化是形成 β-甲氧基-2-呋喃乙醇机理的第一步,其形成的特点是中间体在催化剂表面的重排。
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引用次数: 0
Ruthenium Cluster Decorated Titanium Dioxide Nanowire Arrays for Alkaline Hydrogen Evolution 用于碱性氢气进化的钌簇装饰二氧化钛纳米线阵列
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1007/s10562-024-04857-x
Shipeng Wang, Longrun Sang, Feiyan Zhang, Yongcheng Li, Benhua Xu, Peng Zhang, Bingxin Liu, Yunsi Wang

Enhancing the performance of ruthenium (Ru)-based electrocatalysts for the alkaline hydrogen evolution reaction (HER) presents a significant challenge. Herein, titanium dioxide nanowire arrays decorated with ruthenium clusters were grown on carbon cloth (Ru-TiO2 NWAs/CC) via a two-step hydrothermal method. The nanowire array structure increases the surface area of the substrate, allowing for more Ru clusters to be decorated, thereby improving catalytic activity. The resulting Ru3–TiO2 NWAs/CC catalyst exhibits prominent HER performance in 1.0 M KOH with overpotentials of 61 at 10 mA cm−2 and a Tafel slope of only 47.4 mV dec−1. Furthermore, it maintains outstanding stability under alkaline conditions for more than 10 h. The Ru clusters decoration enhances the TiO2/CC kinetic, more active sites were exposed on nanowires of the surface and accelerated electron transport, thus reducing the charge transfer barrier. After the electrochemical test, the morphology and structure of Ru3–TiO2/CC remained largely unchanged, and the valence states of the elements remained stable. This work paves the road to exploiting highly active and cost-efficient electrocatalysts for alkaline hydrogen evolution.

Graphical Abstract

提高以钌(Ru)为基础的碱性氢气进化反应(HER)电催化剂的性能是一项重大挑战。在此,通过两步水热法在碳布(Ru-TiO2 NWAs/CC)上生长了装饰有钌团簇的二氧化钛纳米线阵列。纳米线阵列结构增加了基底的表面积,从而可以装饰更多的 Ru 簇,从而提高催化活性。所制备的 Ru3-TiO2 NWAs/CC 催化剂在 1.0 M KOH 中表现出卓越的 HER 性能,在 10 mA cm-2 时过电位为 61,Tafel 斜率仅为 47.4 mV dec-1。Ru 簇装饰增强了 TiO2/CC 的动力学性能,更多的活性位点暴露在表面纳米线上,加速了电子传输,从而降低了电荷转移障碍。经过电化学测试,Ru3-TiO2/CC 的形貌和结构基本保持不变,元素的价态也保持稳定。这项工作为开发高活性、低成本的碱性氢气进化电催化剂铺平了道路。
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引用次数: 0
Retraction Note: Co5.47 N/rGO@NF as a High-Performance Bifunctional Catalyst for Urea-Assisted Hydrogen Evolution 撤回声明:Co5.47 N/rGO@NF 作为尿素辅助氢气转化的高性能双功能催化剂
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1007/s10562-024-04879-5
Liqin Yang, Yongli Liu, Lei Wang, Zhiju Zhao, Cuijuan Xing, Shuhe Shi, Meiling Yuan, Zhaoming Ge, Zhenyu Cai
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引用次数: 0
Preparation of Silicon Carbide Supported Iron Catalysts and their Catalytic Activities in Hydrogen Production by Ammonia Decomposition 碳化硅支撑铁催化剂的制备及其在氨分解制氢中的催化活性
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1007/s10562-024-04858-w
Yulian Liu, Fengxiang Yin, Guoru Li, Yuhang Tan

In this study, silicon carbide (SiC) was prepared from sol–gel process combined with subsequent carbothermal reaction. Then through hydrothermal method synthesized xFe/SiC-700 and 30Fe/SiC-T catalysts. The catalysts were characterized by XRD, SEM/TEM, XPS, and H2-TPR. The ammonia decomposition performances of the catalysts were assessed in a fixed-bed reactor. Tests revealed that SiC has a high specific surface area and can evenly diffuse Fe2O3 nanoparticles, thus exposing more active sites and raising the adsorption capacity of catalysts surface. The interaction of Fe2O3 and SiC is stronger, the catalyst activity is better. The surface basicity of catalyst is higher, decomposition ability of ammonia is stronger. 30Fe/SiC-700 catalyst has the best activity among the synthesized catalysts for hydrogen production by ammonia decomposition. The ammonia conversion rate can reach up to 90.16%, and the hydrogen generation can rate reach up to 30.19 mmol·min−1·gcat−1 at 600 °C at 30,000 mL·gcat−1·h−1. Moreover, the catalytic activity is efficient and stable after continuous reaction at 600 °C for 160 h.

Graphical Abstract

Ammonia decomposition: The silicon carbide supported iron oxide catalyst was prepared, which effectively cracked ammonia to produce COX-free H2.

在这项研究中,碳化硅(SiC)是通过溶胶凝胶工艺结合后续的碳热反应制备的。然后通过水热法合成了 xFe/SiC-700 和 30Fe/SiC-T 催化剂。催化剂通过 XRD、SEM/TEM、XPS 和 H2-TPR 进行了表征。在固定床反应器中对催化剂的氨分解性能进行了评估。测试表明,SiC 具有较高的比表面积,可以均匀扩散 Fe2O3 纳米颗粒,从而暴露出更多的活性位点,提高催化剂表面的吸附能力。Fe2O3 与 SiC 的相互作用更强,催化剂活性更好。催化剂的表面碱性更高,氨的分解能力更强。在合成的氨分解制氢催化剂中,30Fe/SiC-700 催化剂的活性最好。在 600 ℃、30,000 mL-gcat-1-h-1 条件下,氨的转化率可达 90.16%,氢的生成率可达 30.19 mmol-min-1-gcat-1。此外,在 600 °C 下连续反应 160 h 后,催化活性高效稳定:制备了碳化硅支撑的氧化铁催化剂,该催化剂能有效裂解氨气生成不含 COX 的 H2。
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引用次数: 0
Unravelling the Synthesis of 2-Aminobenzo[d]thiazole Derivatives via a Novel Zinc(II)-Catalyzed Strategy 通过新型锌(II)催化策略揭示 2-氨基苯并[d]噻唑衍生物的合成过程
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1007/s10562-024-04835-3
Mohan Neetha, S. B. Umabharathi, Gopinathan Anilkumar

The first zinc(II)-catalyzed approach towards an array of 2-aminobenzothiazole derivatives was successfully developed. In this process, the substrate 2-bromophenyl isothiocyanate was reacted with a range of amines, including aromatic and aliphatic (primary and secondary) and cyclic secondary amines, yielding the products in reasonably good amounts. The reactivity analyses of different amines revealed that cyclic secondary amines performed exceptionally well, providing excellent outcomes. Additionally, aliphatic amines also exhibited the capability to undergo the transformation successfully.

Graphical Abstract

首次成功开发出锌(II)催化的 2-氨基苯并噻唑衍生物系列。在这一过程中,底物 2-溴苯基异硫氰酸酯与一系列胺类(包括芳香族和脂肪族(伯胺和仲胺)以及环状仲胺)发生反应,以合理的数量生成产物。对不同胺类的反应性分析表明,环状仲胺的反应性特别好,能产生极佳的结果。此外,脂肪族胺也表现出了成功进行转化的能力。
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引用次数: 0
First Principles Study of Photocatalytic Water Splitting Hydrogen Production by SiI2 Nanotubes 二氧化硅纳米管光催化水分离制氢的第一原理研究
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1007/s10562-024-04870-0
Huanyu Zhao, Hongyu Song, Yingtao Zhu, Chao Wang, Xuan Hui, Long Zhang

We use density functional theory (DFT) to calculate the optimal parameters of atomic arrangement, energy level and electronic structure of sawtooth (n, 0) nanotubes in this paper. The strain energy and formation energy data show that the coiled process of nanotubes is endothermic, and the correlation value decreases with the increase of the radius. Our study shows that the band gap width of SiI2 nanotubes first increases and then decreases with the increase of the nanotube radius. The band gap of SiI2 nanotubes changes from indirect to direct after the single layer is rolled into nanotubes and have appropriate band gaps for absorbing visible light. In addition, it is speculated that the disparity between the effective mass of electrons and holes can reduce charge carrier recombination. Among them, the n value 10 ~ 50 nanotubes showed redox capacity between pH = 7 and 0, and the reducing capacity increased with the increase of tube radius. In conclusion, we believe that SiI2 nanotubes have great application potential in photocatalytic water splitting.

Graphical Abstract

Visible light absorption indicate that SiI2 nanotube should be effective photocatalysis for production of H2 from splitting water

本文采用密度泛函理论(DFT)计算了锯齿(n,0)纳米管的原子排列、能级和电子结构的最佳参数。应变能和形成能数据表明,纳米管的盘绕过程是内热的,相关值随着半径的增大而减小。我们的研究表明,随着纳米管半径的增大,SiI2 纳米管的带隙宽度先增大后减小。单层卷成纳米管后,SiI2 纳米管的带隙由间接带隙变为直接带隙,并具有吸收可见光的适当带隙。此外,据推测,电子和空穴有效质量的差异可以减少电荷载流子的重组。其中,n 值为 10 ~ 50 的纳米管在 pH = 7 和 0 之间显示出氧化还原能力,并且还原能力随着管半径的增加而增加。总之,我们认为 SiI2 纳米管在光催化分水方面具有巨大的应用潜力。 图解 摘要可见光吸收表明 SiI2 纳米管应能有效地光催化分水产生 H2。
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引用次数: 0
Plasma-Synthesized Combined Nitrogen and Cationic Species Doped-MnO2: Impact on Texture, Optical Properties, and Photocatalytic Activity 等离子体合成的掺杂氮和阳离子的二氧化锰:对质地、光学特性和光催化活性的影响
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-11 DOI: 10.1007/s10562-024-04834-4
Franck W. Boyom-Tatchemo, Albert Poupi, François Devred, Elie Acayanka, Georges Kamgang-Youbi, Carmela Aprile, Samuel Laminsi, Eric M. Gaigneaux

This work explored the possibility of doping MnO2 structure simultaneously by cationic (Na+, Mg2+ or K+) and nitrogen species during its synthesis through gliding arc plasma route. Therefore, NaMnO4, Mg(MnO4)2 or KMnO4 precursor has been precipitated via plasmachemical reduction thanks to NO⋅ and NO2 respectively being short and long-lived species generated in plasma plume (gas phase) and plasma post-discharge (liquid phase). Physicochemical characterizations revealed nanostructured NaN–MnO2, MgN–MnO2 and KN–MnO2 respectively with specific surface areas of 36, 110 and 116 m2/g, nitrogen atomic loading at surface of 0.6, 1.0 and 1.5%, and band gap values of 1.20, 1.30 and 1.45 eV. The three precursors with different cationic species allowed different nitrogen loading for their respective plasma-synthesized MnO2, which led to the different values of band gap energy. An increase of the N-loading induced an increase of band gap energy and enlarged the absorption capability of MnO2 from visible light to the UV region. Solar photocatalytic removal of TY revealed bleaching degrees of 53, 97 and 94% respectively for NaN–MnO2, MgN–MnO2 and KN–MnO2 materials. This enlargement, together with the increased specific surface area of the plasma-synthesized N–MnO2, led synergistically to an enhancement of its photocatalytic activity. This work highlights the usefulness of the synthesis via glidarc plasma, without any additional reagent, of MnO2, as allowing cationic species insertion in their structure, and simultaneously their doping with different N-loading, so leading to different crystalline structures, and photocatalytic activities.

Graphical Abstract

这项研究探索了在通过滑弧等离子体途径合成 MnO2 的过程中同时掺入阳离子(Na+、Mg2+ 或 K+)和氮元素的可能性。因此,NaMnO4、Mg(MnO4)2 或 KMnO4 前驱体通过等离子体化学还原沉淀,而 NO⋅ 和 NO2- 分别是等离子体羽流(气相)和等离子体放电后(液相)中产生的短寿命和长寿命物种。物理化学特征显示,纳米结构的 NaN-MnO2、MgN-MnO2 和 KN-MnO2 的比表面积分别为 36、110 和 116 m2/g,表面氮原子负载分别为 0.6、1.0 和 1.5%,带隙值分别为 1.20、1.30 和 1.45 eV。具有不同阳离子种类的三种前驱体可使各自等离子体合成的二氧化锰具有不同的氮负荷,从而导致不同的带隙能值。氮负载量的增加会导致带隙能的增加,并使二氧化锰的吸收能力从可见光扩大到紫外区。太阳能光催化去除 TY 的结果显示,NaN-MnO2、MgN-MnO2 和 KN-MnO2 材料的漂白度分别为 53%、97% 和 94%。这种扩大与等离子体合成的 N-MnO2 比表面积的增加一起,协同增强了其光催化活性。这项工作凸显了通过滑弧等离子体合成 MnO2 的实用性,无需任何额外试剂,就能在其结构中插入阳离子物种,同时掺入不同的 N 负荷,从而产生不同的晶体结构和光催化活性。
{"title":"Plasma-Synthesized Combined Nitrogen and Cationic Species Doped-MnO2: Impact on Texture, Optical Properties, and Photocatalytic Activity","authors":"Franck W. Boyom-Tatchemo,&nbsp;Albert Poupi,&nbsp;François Devred,&nbsp;Elie Acayanka,&nbsp;Georges Kamgang-Youbi,&nbsp;Carmela Aprile,&nbsp;Samuel Laminsi,&nbsp;Eric M. Gaigneaux","doi":"10.1007/s10562-024-04834-4","DOIUrl":"10.1007/s10562-024-04834-4","url":null,"abstract":"<div><p>This work explored the possibility of doping MnO<sub>2</sub> structure simultaneously by cationic (Na<sup>+</sup>, Mg<sup>2+</sup> or K<sup>+</sup>) and nitrogen species during its synthesis through gliding arc plasma route. Therefore, NaMnO<sub>4</sub>, Mg(MnO<sub>4</sub>)<sub>2</sub> or KMnO<sub>4</sub> precursor has been precipitated via plasmachemical reduction thanks to NO⋅ and NO<sub>2</sub><sup>−</sup> respectively being short and long-lived species generated in plasma plume (gas phase) and plasma post-discharge (liquid phase). Physicochemical characterizations revealed nanostructured NaN–MnO<sub>2</sub>, MgN–MnO<sub>2</sub> and KN–MnO<sub>2</sub> respectively with specific surface areas of 36, 110 and 116 m<sup>2</sup>/g, nitrogen atomic loading at surface of 0.6, 1.0 and 1.5%, and band gap values of 1.20, 1.30 and 1.45 eV. The three precursors with different cationic species allowed different nitrogen loading for their respective plasma-synthesized MnO<sub>2</sub>, which led to the different values of band gap energy. An increase of the N-loading induced an increase of band gap energy and enlarged the absorption capability of MnO<sub>2</sub> from visible light to the UV region. Solar photocatalytic removal of TY revealed bleaching degrees of 53, 97 and 94% respectively for NaN–MnO<sub>2</sub>, MgN–MnO<sub>2</sub> and KN–MnO<sub>2</sub> materials. This enlargement, together with the increased specific surface area of the plasma-synthesized N–MnO<sub>2</sub>, led synergistically to an enhancement of its photocatalytic activity. This work highlights the usefulness of the synthesis via glidarc plasma, without any additional reagent, of MnO<sub>2</sub>, as allowing cationic species insertion in their structure, and simultaneously their doping with different N-loading, so leading to different crystalline structures, and photocatalytic activities.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 1","pages":""},"PeriodicalIF":2.3,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598983","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sonochemical Synthesis of Ti1−x−yFexPbyO2 (with x and y = 0, 0.01, 0.03, 0.07): Structural Analysis, Influence of Radiation Type on Photocatalytic Activity and Assessment of Antimicrobial Properties 声化学合成 Ti1-x-yFexPbyO2(x 和 y = 0、0.01、0.03、0.07):结构分析、辐射类型对光催化活性的影响以及抗菌性能评估
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-09 DOI: 10.1007/s10562-024-04841-5
D. F. S. Morais, O. B. M. Ramalho, N. F. Andrade Neto, M. D. Teodoro, K. N. Matsui, M. R. D. Bomio, F. V. Motta

In this work, we report a method of obtaining and characterizing (Fe, Pb) co-doped titanium oxide nanoparticles to study the influence of Fe3+ and Pb2+ doping on the photocatalytic and antimicrobial properties of TiO2. The presence of dopant elements can provide electronic changes by promoting a decrease in the band gap or creating intra-band gap states, thereby allowing greater absorption under visible light irradiation and potentially increasing the efficiency for developing photocatalytic and antimicrobial applications. Therefore, co-doped Ti1−x−yFexPbyO2 (x and y = 0, 0.01, 0.03, 0.07 mol) powders were successfully obtained in a single step by the sonochemical method (SM). The structural, morphological and optical properties were evaluated using X-ray diffraction (XRD), transmission electron microscopy (TEM), Field Emission Gun—Scanning Electron Microscopy (SEM-FEG) and UV–Visible spectroscopy (UV–Vis) techniques. The results showed the successful formation of the anatase phase of (Fe, Pb) co-doped TiO2 by the SM with nanometric particles of irregular morphology. The photoluminescence exhibited low intensity for the co-doped samples, indicating a decrease in the recombination rate of the e−/h + electronic pair, which contributes to the photocatalytic efficiency. Optical measurements revealed a decrease in the band gap, providing possible energetic activation of these semiconductors by sunlight. The photocatalytic activity was estimated through the methylene blue dye (MB) degradation when exposed to UV light and Sunlight, and revealed that the type of radiation used to activate the photocatalysts influences the catalytic activity: T1F (Ti0.99Fe0.01O2) and T1P (Ti0.99Pb0.01O2) samples degraded the dye by 50% and 65% under UV light for 120 min, respectively, while the degradation under Solar irradiation was 98% and 99%, respectively. Antimicrobial properties were also investigated by agar diffusion method against E. coli (gram-negative) and S. aureus (gram-positive) bacteria and showed positive results of (Fe, Pb) co-doped TiO2 samples compared to pure TiO2. Accordingly, the results indicate that the co-doping of TiO2 with Fe3+ and Pb2+ influences its potential application as photocatalysts and antimicrobial agents.

Graphical Abstract

在这项工作中,我们报告了一种获得和表征(Fe、Pb)共掺杂氧化钛纳米粒子的方法,以研究掺杂 Fe3+ 和 Pb2+ 对二氧化钛光催化和抗菌特性的影响。掺杂元素的存在可通过促进带隙的减小或产生带隙内态来实现电子变化,从而在可见光照射下实现更大的吸收,并有可能提高光催化和抗菌应用的开发效率。因此,采用声化学法(SM)一步法成功地获得了共掺杂 Ti1-x-yFexPbyO2(x 和 y = 0、0.01、0.03、0.07 摩尔)粉末。利用 X 射线衍射(XRD)、透射电子显微镜(TEM)、场发射枪扫描电子显微镜(SEM-FEG)和紫外可见光谱(UV-Vis)技术对粉末的结构、形态和光学性质进行了评估。结果表明,通过 SM 成功地形成了(铁、铅)共掺杂 TiO2 的锐钛矿相,并具有形态不规则的纳米颗粒。共掺杂样品的光致发光强度较低,表明 e-/h + 电子对的重组率降低,这有助于提高光催化效率。光学测量显示带隙减小,这说明这些半导体可能被阳光激活。光催化活性是通过亚甲基蓝染料(MB)在紫外线和日光照射下的降解进行估算的,结果表明,用于激活光催化剂的辐射类型会影响催化活性:T1F(Ti0.99Fe0.01O2)和 T1P(Ti0.99Pb0.01O2)样品在紫外线照射下 120 分钟的染料降解率分别为 50%和 65%,而在太阳光照射下的降解率分别为 98%和 99%。此外,还采用琼脂扩散法对大肠杆菌(革兰氏阴性)和金黄色葡萄球菌(革兰氏阳性)进行了抗菌性能研究,结果表明,与纯 TiO2 相比,(铁、铅)共掺杂 TiO2 样品具有良好的抗菌性能。因此,研究结果表明,TiO2 与 Fe3+ 和 Pb2+ 的共掺杂影响了其作为光催化剂和抗菌剂的潜在应用。
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引用次数: 0
Study on Effect of Calcination and Ag Loading on Ag/TiO2 Catalyst for Low-Temperature Selective Catalytic Oxidation of Ammonia 氨的低温选择性催化氧化中 Ag/TiO2 催化剂的煅烧和银负载效应研究
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-09 DOI: 10.1007/s10562-024-04833-5
Bin Guan, Junyan Chen, Zhongqi Zhuang, Lei Zhu, Zeren Ma, Xuehan Hu, Chenyu Zhu, Sikai Zhao, Kaiyou Shu, Hongtao Dang, Tiankui Zhu, Zhen Huang

Herein, Ag/TiO2 NH3-SCO catalyst was prepared by impregnation-rotary evaporation method with different calcination temperature and Ag loading content. The results of performance evaluation and characterization showed that the 10 wt% Ag/TiO2 catalyst calcined at 500 °C showed the best comprehensive performance, with T99 reaching 175 °C and N2 selectivity reaching 80% at high temperatures. High-temperature calcination will lead to a significant decline in catalyst activity, accompanied by the transformation of TiO2 from anatase to rutile phase and the obvious change and loss of Ag active sites, which greatly reduces the NH3 adsorption and redox ability, but it can still maintain a high N2 selectivity due to unchanged reaction mechanism. In addition, with the increase of Ag loading, excess Ag on Ag/TiO2 will form metal clusters due to the lack of sufficient anchor points, which helps to improve NH3-SCO activity. However, excessive Ag loading will reduce the specific surface area and acidic sites, and the Ag species on the catalyst surface will also change to the form of larger particles of Ag2O, which will lead to the decline of catalytic performance.

Graphical Abstract

本文采用浸渍-旋转蒸发法制备了不同煅烧温度和Ag负载量的Ag/TiO2 NH3-SCO催化剂。性能评价和表征结果表明,在 500 ℃ 下煅烧的 10 wt% Ag/TiO2 催化剂综合性能最好,高温下 T99 达到 175 ℃,N2 选择性达到 80%。高温煅烧会导致催化剂活性显著下降,伴随着 TiO2 由锐钛相转变为金红石相,Ag 活性位点发生明显变化和损失,从而大大降低了 NH3 的吸附和氧化还原能力,但由于反应机理不变,仍能保持较高的 N2 选择性。此外,随着 Ag 负载的增加,Ag/TiO2 上过量的 Ag 会因缺乏足够的锚点而形成金属簇,这有助于提高 NH3-SCO 活性。但是,过量的 Ag 负载会降低比表面积和酸性位点,催化剂表面的 Ag 物种也会转变为较大颗粒的 Ag2O,从而导致催化性能下降。
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引用次数: 0
Microscopic Investigation of CO Oxidation Reaction by Copper–Manganese Oxide Catalysts 铜锰氧化物催化剂对一氧化碳氧化反应的显微研究
IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-11-09 DOI: 10.1007/s10562-024-04846-0
Zhaoyue He, Bin Zheng

The catalytic oxidation of CO is a significant process for environmental and human health protection. The CuMnOx (hopcalite) catalyst is a good candidate for the CO oxidation reaction, owing to advantages such as low cost and good catalytic activity at low temperature. In this study, a combination of reactive force field molecular dynamic simulations and density functional theory calculations was employed to investigate the CO oxidation reaction catalyzed by CuMnOx. We examined the effect of three factors (oxygen content of CuMnOx catalyst, pressure, and free O2 concentration) on enhancing the CO conversion. The CuMnO4 catalyst exhibited superior performance in the CO oxidation reaction. The main oxygen source of the oxidation product (CO2) was found to be the lattice oxygen atoms of the CuMnOx catalyst. The energy barrier of the oxidation reaction between CO and the lattice oxygens was relatively low, showing that this reaction was kinetically favored. The present results provide microscopic insight into the CO oxidation reaction catalyzed by CuMnOx, which is expected to elucidate the corresponding mechanism and thus guide the design of highly active catalysts.

Graphical Abstract

一氧化碳的催化氧化是保护环境和人类健康的重要过程。CuMnOx(hopcalite)催化剂具有成本低、低温催化活性好等优点,是 CO 氧化反应的理想候选催化剂。本研究结合反应力场分子动力学模拟和密度泛函理论计算,研究了 CuMnOx 催化的 CO 氧化反应。我们考察了三个因素(CuMnOx 催化剂的氧含量、压力和游离 O2 浓度)对提高 CO 转化率的影响。CuMnO4 催化剂在 CO 氧化反应中表现出更优越的性能。研究发现,氧化产物(CO2)的主要氧源是 CuMnOx 催化剂的晶格氧原子。CO 与晶格氧原子之间的氧化反应能垒相对较低,表明这一反应在动力学上是有利的。本研究结果从微观上揭示了 CuMnOx 催化的 CO 氧化反应,有望阐明相应的机理,从而指导高活性催化剂的设计。
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引用次数: 0
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Catalysis Letters
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