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Rational design of aqueous tertiary amine solvent for integrated CO2 capture and hydrogenation 二氧化碳捕获和氢化一体化叔胺水溶液的合理设计
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-02-08 DOI: 10.1016/j.catcom.2024.106866
Zhi-Gang Hu , Lichun Li , Shui-Bao Yu , Zhengfei Chen , Jian-Quan Weng

Several tertiary amine solutions with different structures were tested in the integrated CO2 capture and hydrogenation process in the presence of heterogeneous Pd/NAC catalysts. The tertiary amines of 3-dimethylamino-1,2-propanediol (3DMA-1,2-PD) and 3-diethylamino-1,2-propanedio (3DEA-1,2-PD) with high CO2 absorption capacity and high formate yield were selected as suitable candidates as CO2 capture and hydrogenation solvents. Under mild reaction conditions, a high formate yield of 68% was achieved when using 1 M 3DMA-1,2-PD solution with CO2 loading of 0.5 mol amine/mol CO2. In addition, the physico-chemical properties of the Pd/NAC catalysts were examined and the reaction mechanism of CO2 absorption and hydrogenation in the presence of Pd/NAC was proposed.

在异相钯/NAC 催化剂存在下的二氧化碳捕获和加氢一体化过程中,对几种不同结构的叔胺溶液进行了测试。3-二乙氨基-1,2-丙二醇(3DMA-1,2-PD)和 3-二乙氨基-1,2-丙二醇(3DEA-1,2-PD)的叔胺具有高二氧化碳吸收能力和高甲酸盐产率,被选为二氧化碳捕获和加氢溶剂的合适候选物质。在温和的反应条件下,当使用 1 M 3DMA-1,2-PD 溶液且二氧化碳负载量为 0.5 摩尔胺/摩尔二氧化碳时,甲酸酯产率高达 68%。此外,还研究了 Pd/NAC 催化剂的物理化学性质,并提出了 Pd/NAC 存在下二氧化碳吸收和加氢的反应机理。
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引用次数: 0
Nb2O5/MWCNT nanocomposites for the degradation of ibuprofen via photocatalysis and catalytic ozonation 通过光催化和催化臭氧降解布洛芬的 Nb2O5/MWCNT 纳米复合材料
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-01-20 DOI: 10.1016/j.catcom.2024.106853
Michel Z. Fidelis , Ana S.G.G. dos Santos , Elaine T. de Paula , Giane G. Lenzi , Olivia S.G.P. Soares , Onelia A.B. Andreo

Growing concerns regarding the inefficient degradation of persistent pollutants, such as ibuprofen, in water necessitate the development of advanced treatment methods. Nb2O5, with its properties resembling those of TiO2, emerges as a promising alternative catalyst for advanced catalytic treatments. In this work, we demonstrate the exceptional catalytic ozonation and photocatalysis performance of Nb2O5/MWCNT nanocomposites synthesized via three sol-gel methods. These composites achieve complete ibuprofen degradation within 30 min, outperforming conventional catalysts and ozonation alone due to their enhanced surface area and synergistic interactions. Nb2O5/MWCNT presents a compelling solution, offering an efficient and sustainable approach to water purification.

人们日益关注水中持久性污染物(如布洛芬)降解效率低下的问题,因此有必要开发先进的处理方法。Nb2O5 具有与 TiO2 相似的特性,有望成为先进催化处理的替代催化剂。在这项工作中,我们展示了通过三种溶胶-凝胶方法合成的 Nb2O5/MWCNT 纳米复合材料的优异臭氧催化和光催化性能。这些复合材料在 30 分钟内实现了布洛芬的完全降解,其性能优于传统催化剂和单独的臭氧催化,这得益于它们增强的比表面积和协同作用。Nb2O5/MWCNT 是一种引人注目的解决方案,为水净化提供了一种高效、可持续的方法。
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引用次数: 0
Green synthesis of ZnO photocatalyst composited carbon quantum dots (CQDs) from lime (Citrus aurantifolia) 从酸橙(Citrus aurantifolia)中绿色合成 ZnO 光催化剂复合碳量子点 (CQDs)
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-02-27 DOI: 10.1016/j.catcom.2024.106888
Rizky Nur Hidayat , Hendri Widiyandari , Hanaiyah Parasdila , Orien Prilita , Yayuk Astuti , Nandang Mufti , Takashi Ogi

Lime (Citrus aurantifolia) is one of the most extensively exported agricultural products from Indonesia. Citric acid and ascorbic acid content from limes (Citrus aurantifolia) is such one of the carbon-rich fruits that is a suitable source for Carbon Quantum Dots (CQDs) synthesis. CQD synthesized by relying on natural carbon precursors from lime (Citrus aurantifolia) is a more environmentally friendly approach in the present research, CQDs in this research will be used as an addition to ZnO by hydrothermal method in order to enhance photocatalytic activity. Corresponding to the results, the presence of CQDs improves both the optical and structural properties of ZnO, which led to enhance photocatalytic activity with a degradation percentage of 98% shortly after 75 min of visible light irradiation and to each of the repeatability test cycle results showing the consistent results and with the rate constant (k) fluctuating and the specified compound's degradation percentage remains relatively constant with minor changes.

莱姆()是印度尼西亚出口量最大的农产品之一。石灰()中的柠檬酸和抗坏血酸是富含碳的水果之一,是合成碳量子点(CQDs)的合适来源。在本研究中,CQDs 将通过水热法作为 ZnO 的添加剂,以增强光催化活性。结果表明,CQDs 的存在改善了 ZnO 的光学和结构特性,从而提高了光催化活性,在可见光照射 75 分钟后,降解率达到 98%。
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引用次数: 0
Opportunities and limitations of metal additive manufacturing of structured catalytic converters 结构化催化转化器金属添加剂制造的机遇和局限性
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-02-15 DOI: 10.1016/j.catcom.2024.106873
Fatemeh Mehdipour , Tim Delrieux , Florian Maurer , Jan-Dierk Grunwaldt , Christoph Klahn , Roland Dittmeyer

Utilising additive manufacturing (AM), reactors with composite structures, featuring locally tuned geometries and controlled porosity, can effectively be employed in chemical reactions. This innovation yields enhancements in flow and transport properties across both axial and transverse dimensions. Integrating structured catalysts with AM offers great potentials, albeit faces notable challenges. A significant challenge is scarce availability of suitable high-temperature materials for AM of catalytic converters. Furthermore, ensuring optimal adhesion and chemical interactions between catalyst systems and printed materials necessitates detailed investigations. This paper examines advantages and challenges associated with AM of structured catalytic converters, employing emission control systems as an illustration.

利用增材制造(AM)技术,具有复合结构的反应器可以有效地用于化学反应,其特点是局部调整几何形状和控制孔隙率。这种创新可提高轴向和横向的流动和传输性能。将结构催化剂与 AM 相结合具有巨大的潜力,但也面临着显著的挑战。一个重要的挑战是,用于催化转换器 AM 的合适高温材料非常稀缺。此外,要确保催化剂系统与印刷材料之间的最佳粘附性和化学作用,还需要进行详细的研究。本文以排放控制系统为例,探讨了与结构化催化转换器 AM 相关的优势和挑战。
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引用次数: 0
Preparation of core-shell Ni/CeO2@Al2O3 catalyst for selective hydrogenation of acetylene 制备用于乙炔选择性加氢的核壳 Ni/CeO2@Al2O3 催化剂
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.catcom.2024.106860
Zhichao Na , Liuyi Pan , Hedan Yao , Liang Chen , Yanhui Liu , Jiaojiao Liu , Zihao Tao , Dong Li , Wenhong Li

Lattice strain and ligand effects of core-shell structure regulate the geometric and electronic properties of the active metal on the surface of catalysts. Herein, a core-shell Ni/CeO2@Al2O3 catalyst was prepared by hydrothermal deposition for selective hydrogenation of acetylene. Compared with the general Ni/Al2O3 catalyst, the ethylene selectivity of the Ni/CeO2@Al2O3 catalyst was significantly improved due to the special structure reduced the adsorption strength of ethylene. Under the condition of 10% CeO2 loading, the performance of the catalyst was the best (85.3% C2H2 conversion and 81.2% C2H4 selectivity). This work provided a new approach for exploring efficient catalysts for semi‑hydrogenation reaction.

核壳结构的晶格应变和配体效应可调节催化剂表面活性金属的几何和电子特性。本文采用水热沉积法制备了一种核壳 Ni/CeO2@Al2O3 催化剂,用于乙炔的选择性加氢反应。与一般的 Ni/Al2O3 催化剂相比,Ni/CeO2@Al2O3 催化剂的乙烯选择性显著提高,原因在于其特殊的结构降低了对乙烯的吸附强度。在 CeO2 加载 10% 的条件下,催化剂的性能最好(C2H2 转化率为 85.3%,C2H4 选择性为 81.2%)。这项工作为探索半加氢反应的高效催化剂提供了一种新方法。
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引用次数: 0
H2 production by solar photoreforming of plastic materials using SiC-g-C3N4composites 利用 SiC-g-C3N4 复合材料对塑料材料进行太阳能光致转化生产 H2
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-01-17 DOI: 10.1016/j.catcom.2024.106850
Maria Teresa Armeli Iapichino , Roberto Fiorenza , Vincenzo Patamia , Giuseppe Floresta , Antonino Gulino , Marcello Condorelli , Giuliana Impellizzeri , Giuseppe Compagnini , Salvatore Sciré

The photoreforming of polyethylene terephthalate and bisphenol A was here investigated using uncommon photocatalysts (SiC-g-C3N4 composites). The results showed as the addition of small amounts of g-C3N4 on SiC promoted an efficient charge carriers separation and a good interaction between the two materials, leading to a H2 production rate of 18 and 12 μmolH2/gcat∙h for the photoreforming of polyethylene terephthalate and bisphenol A, respectively. The accurate selection of different g-C3N4 precursors, combined with the appropriate control of the key reaction parameters (pH and plastic materials pretreatments) allowed to optimize the performance of the SiC-g-C3N4 composites for the photocatalytic H2 production.

本文使用不常见的光催化剂(SiC-g-C3N4 复合材料)研究了聚对苯二甲酸乙二醇酯和双酚 A 的光转化。结果表明,在 SiC 上添加少量 g-C3N4 可促进电荷载流子的有效分离以及两种材料之间的良好相互作用,从而使聚对苯二甲酸乙二醇酯和双酚 A 的光致转化率分别达到 18 μmolH2/gcat∙h 和 12 μmolH2/gcat∙h。准确选择不同的 g-C3N4 前体,结合适当控制关键反应参数(pH 值和塑料材料预处理),可以优化 SiC-g-C3N4 复合材料光催化产生 H2 的性能。
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引用次数: 0
Photochemical transformation of UiO-66-NH2 during hydrogen generation under solar irradiation 太阳照射下制氢过程中 UiO-66-NH2 的光化学转化
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-01-30 DOI: 10.1016/j.catcom.2024.106858
Lorena Gudiño, Manuel Peñas-Garzón, Juan J. Rodriguez, Jorge Bedia, Carolina Belver

This work reports for the first time the photochemical transformation suffered by the UiO-66-NH2 MOF during hydrogen production under solar irradiation using different scavengers. Triethanolamine caused the complete dissolution of the MOF, while Na2S/Na2SO3 transformed the UiO-66-NH2 into a novel Zr-based material characterized by an amorphous structure with a production rate of 0.439 μmol H2·gcat−1·h−1. The MOF-derived material maintained its performance during long-term on-stream experiments thanks to the electron transfer from the sulfide/sulfite ions to the valence band of the photocatalyst. However, significant doubts about the stability of UiO-66NH2 and other MOFs in the photocatalytic generation of hydrogen are arisen.

这项研究首次报道了 UiO-66-NH2 MOF 在太阳辐照下利用不同的清除剂制氢过程中发生的光化学转变。三乙醇胺导致 MOF 完全溶解,而 Na2S/Na2SO3 则将 UiO-66-NH2 转化为一种新型 Zr 基材料,该材料具有无定形结构,制氢率为 0.439 μmol H2-gcat-1-h-1。由于电子从硫化物/亚硫酸根离子转移到光催化剂的价带,MOF 衍生材料在长期在线实验中保持了其性能。然而,人们对 UiO-66NH2 和其他 MOF 在光催化制氢过程中的稳定性产生了极大的怀疑。
{"title":"Photochemical transformation of UiO-66-NH2 during hydrogen generation under solar irradiation","authors":"Lorena Gudiño,&nbsp;Manuel Peñas-Garzón,&nbsp;Juan J. Rodriguez,&nbsp;Jorge Bedia,&nbsp;Carolina Belver","doi":"10.1016/j.catcom.2024.106858","DOIUrl":"10.1016/j.catcom.2024.106858","url":null,"abstract":"<div><p>This work reports for the first time the photochemical transformation suffered by the UiO-66-NH<sub>2</sub> MOF during hydrogen production under solar irradiation using different scavengers. Triethanolamine caused the complete dissolution of the MOF, while Na<sub>2</sub>S/Na<sub>2</sub>SO<sub>3</sub> transformed the UiO-66-NH<sub>2</sub> into a novel Zr-based material characterized by an amorphous structure with a production rate of 0.439 μmol H<sub>2</sub>·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup>. The MOF-derived material maintained its performance during long-term on-stream experiments thanks to the electron transfer from the sulfide/sulfite ions to the valence band of the photocatalyst. However, significant doubts about the stability of UiO-66NH<sub>2</sub> and other MOFs in the photocatalytic generation of hydrogen are arisen.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106858"},"PeriodicalIF":3.7,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000189/pdfft?md5=37d80d2d01a5ffe2798f585c5847a3c5&pid=1-s2.0-S1566736724000189-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139578071","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
A facile synthesis of hierarchical Nanosized zeolite Beta and its application in direct crude oil hydrocracking 分层纳米沸石 Beta 的简易合成及其在原油直接加氢裂化中的应用
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-02-10 DOI: 10.1016/j.catcom.2024.106871
Faisal M. Alotaibi , Lianhui Ding , Husin Sitepu , Qasim Saleem , Donya A. Alsewdan , Anaam Shaikh Ali , Sakinah I. Bin Hamad , Meshary H. Alotaibi , Mohammad F. Aljishi

This study focuses on the synthesis of hierarchical nano-sized beta zeolites that exhibit enhanced catalytic properties through zeolite particle size reduction (to <80 nm) and the introduction of mesopores inside and between particles to improve diffusion of large molecules. The zeolites were produced by desilication and with template-including nano-sized beta as starting material. The samples were characterized by BET, XRD, XRF, solid-state NMR, TG-DTA, and NH3-TPD. Our method uses a shortened synthesis process to yield zeolites with higher surface area, pore volume (>1.0 ml/g), and stronger acidity that those developed by other methods. The zeolite reaction performances were evaluated in crude oil hydrocracking under commercial hydrocracker operating conditions in a pilot plant unit. The testing results showed that the catalyst including the hierarchical nanosized zeolite beta had much higher heavy oil conversion activity and naphtha selectivity.

本研究的重点是合成分层纳米级贝塔沸石,通过缩小沸石颗粒尺寸(至 80 纳米),并在颗粒内部和颗粒之间引入介孔以改善大分子的扩散,从而增强沸石的催化性能。这些沸石是以包括纳米级贝塔在内的模板为起始材料,通过脱硅法生产出来的。样品通过 BET、XRD、XRF、固态 NMR、TG-DTA 和 NH3-TPD 进行了表征。与其他方法相比,我们的方法缩短了合成过程,得到的沸石具有更高的比表面积、孔隙率(1.0 ml/g)和更强的酸性。在中试装置的商业加氢裂化操作条件下,对沸石在原油加氢裂化中的反应性能进行了评估。测试结果表明,包括分层纳米沸石 beta 在内的催化剂具有更高的重油转化活性和石脑油选择性。
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引用次数: 0
An S-scheme heterojunction BiOBr QDs/Bi7O9I3 nanoflowers enabling enhanced photocatalytic oxygen evolution 可增强光催化氧进化的 S 型异质结 BiOBr QDs/Bi7O9I3 纳米花束
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-01-11 DOI: 10.1016/j.catcom.2024.106843
Qian Li , Xin Pan , Xingguo Wang , Chengbing Ma , Jitang Chen , Yan Han , Biao Wang , Lianzhen Bo , Huiquan Li , Xinying Liu , Yupeng Yuan

Constructing a heterojunction is an effective strategy to achieve high-efficiency separation of charges, which enhances the photocatalytic performance. Here, we present a 0D/3D S-scheme heterojunction, BiOBr/Bi7O9I3, which was constructed by incorporating highly dispersed BiOBr quantum dots (QDs) onto the surface of Bi7O9I3 nanoflowers. This heterostructure effectively absorbs visible light and enhances the separation of charge carriers significantly via an S-scheme pathway. As a result, the BiOBr/Bi7O9I3 photocatalysts demonstrated an excellent photocatalytic O2 evolution rate, achieving a rate of nearly 1500 μmol h−1 g−1. This work highlights the effectiveness of constructing S-scheme heterojunctions to enhance photocatalytic O2 evolution.

构建异质结是实现高效电荷分离、提高光催化性能的有效策略。在这里,我们介绍了一种 0D/3D S 型异质结 BiOBr/Bi7O9I3,它是通过在 Bi7O9I3 纳米花表面加入高度分散的 BiOBr 量子点(QDs)而构建的。这种异质结构能有效吸收可见光,并通过 S 型途径显著增强电荷载流子的分离。因此,BiOBr/Bi7O9I3 光催化剂表现出卓越的光催化 O2 演化率,达到近 1500 μmol h-1 g-1。这项工作凸显了构建 S 型异质结以提高光催化 O2 演化的有效性。
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引用次数: 0
Stability, deactivation and regeneration study of a newly developed HZSM-5 and Ni-doped HZSM-5 zeolite catalysts for ethanol-to-hydrocarbon conversion 新研制的HZSM-5和ni掺杂HZSM-5分子筛乙醇制烃催化剂的稳定性、失活和再生研究
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-01-01 Epub Date: 2023-11-15 DOI: 10.1016/j.catcom.2023.106802
Ifeanyi Michael Smarte Anekwe , Maggie Chetty , Lindiwe Khotseng , Sammy Lewis Kiambi , Lakesh Maharaj , Bilainu Oboirien , Yusuf Makarfi Isa

This work investigates the stability and regeneration of HZSM-5 and Ni/HZSM-5 catalysts in the ethanol-to-hydrocarbon conversion. The catalysts were characterised using different techniques and evaluated at 623 K and 7 h−1 for 96 h TOS with two regeneration cycles. HZSM-5 showed high stability with 100% ethanol conversion, while Ni/HZSM-5 catalysts maintained 100% stability for 48 h before dropping. Regenerated catalysts were comparable to the originals in terms of product distribution, stability, and performance. HZSM-5 preferred BTX, while Ni-doped catalysts favoured C5-C8, C9-C12, and C12+ synthesis. The regeneration process restored catalytic activity, especially for the Ni-doped catalysts, extending their life and reducing replacement costs.

研究了HZSM-5和Ni/HZSM-5催化剂在乙醇制烃过程中的稳定性和再生能力。采用不同的技术对催化剂进行了表征,并在623 K和7 h−1下对96 h TOS进行了两次再生循环。HZSM-5在100%乙醇转化率下表现出较高的稳定性,而Ni/HZSM-5催化剂在48 h内保持100%的稳定性。再生催化剂在产品分布、稳定性和性能方面与原催化剂相当。HZSM-5有利于BTX的合成,而ni掺杂催化剂有利于C5-C8、C9-C12和C12+的合成。再生过程恢复了催化活性,特别是镍掺杂催化剂,延长了它们的寿命并降低了更换成本。
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引用次数: 0
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