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Pt-doped MnOx/AC catalyst for enhanced catalytic performance of formaldehyde at ambient temperature pt掺杂MnOx/AC催化剂在室温下提高甲醛的催化性能
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-09 DOI: 10.1007/s11164-025-05801-3
Liang Li, Dan Xiao, Ran Wang, Zunzhu Xu, Jiwen Zhang, Xiaoxian Jin, Weiwei Zou, Zhaoyang Lu, Beibei Liu

Coating Manganese oxide (MnOx) onto solid substrates is one of the most effective approaches for addressing the inherent agglomeration tendency of powdered MnOx in practical applications. In this study, we deposited MnOx onto activated carbon (AC) and improved the catalytic performance for formaldehyde (HCHO) removal by introducing metal platinum (Pt). When evaluated as catalysts in the HCHO catalytic reaction at ambient temperature, the obtained 0.05 wt% Pt-MnOx/AC catalyst possessed remarkable catalytic and adsorption activity and stability. It could achieve 98%HCHO removal by degrading 1.01 ppm HCHO to 0.02 ppm (0.024 mg/m3) within 2 h in static test at ambient temperature. Further structure-performance investigations revealed the crucial role of metal Pt, which not only improved the oxygen activation capacity but also increased the contents of adsorbed oxygen species and enriched oxygen vacancies; therefore, key intermediates, including performic acid, formate, and CO, can be easily converted. More importantly, the deactivated catalyst regained its full activity after 6 h of air exposure, which was attributed to the rapid regeneration of surface hydroxyl groups through atmospheric O2 and the oxidation of accumulated intermediates. This study reveals the HCHO catalytic mechanism over Pt-MnOx/AC and provides valuable insights into the design of high-activity, relatively low-cost environmental catalysts.

Graphical abstract

在固体衬底上涂覆氧化锰是解决粉末氧化锰固有团聚倾向的最有效方法之一。在本研究中,我们将MnOx沉积在活性炭(AC)上,并通过引入金属铂(Pt)来提高其对甲醛(HCHO)的催化性能。在室温条件下作为HCHO催化反应的催化剂进行评价,得到的0.05 wt% Pt-MnOx/AC催化剂具有良好的催化吸附活性和稳定性。常温下静态试验2 h,将1.01 ppm的HCHO降解为0.02 ppm (0.024 mg/m3), HCHO去除率达98%。进一步的结构性能研究揭示了金属Pt的重要作用,它不仅提高了氧活化能力,而且增加了吸附氧的含量和富氧空位;因此,关键的中间体,包括甲酸、甲酸和一氧化碳,可以很容易地转化。更重要的是,失活的催化剂在暴露于空气6小时后恢复了全部活性,这是由于大气中的O2快速再生了表面羟基,并氧化了积累的中间体。本研究揭示了HCHO在Pt-MnOx/AC上的催化机理,为设计高活性、相对低成本的环境催化剂提供了有价值的见解。图形抽象
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引用次数: 0
Tailored Al-doped ZnO/rGO nanocomposites for enhanced anticancer and photocatalytic activities: a green synthesis approach 用于增强抗癌和光催化活性的定制al掺杂ZnO/rGO纳米复合材料:绿色合成方法
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-08 DOI: 10.1007/s11164-025-05790-3
Zabn Allah M. Alaizeri, Syed Mansoor Ali, Hisham A. Alhadlaq

Owing to their distinctive and tunable physicochemical properties, zinc oxide (ZnO) nanoparticles (NPs) have attracted significant attention in cancer therapy as well as photocatalytic applications. The novelty in this work was to use a green approach using pomegranate peel extract to synthesize pure ZnO NPs, Al-doped ZnO NPs, and Al-ZnO/rGO NCs to improve their photocatalytic and anticancer performance. The synthesized materials were characterized in detail by XRD, SEM, EDX, XPS, FTIR, PL, and DLS. XRD results confirmed the high crystallinity of ZnO and indicated increased crystallite size from 17.60 nm to 21.51 nm by doping and rGO incorporation. The SEM image of ZnO NPs showed spherical shapes with uniform distribution on the surface of rGO. EDX verified the existence of Zn, O, Al, and C in the nanocomposites without observable impurities, whereas XPS revealed the elemental composition and oxidation states. FTIR also supported the presence of functional groups, and UV–Vis results showed a decrease in the bandgap energy from 3.34 eV to 3.25 eV due to doping as well as rGO integration. Based on the PL data, it was supposed that better charge separation and improved photocatalytic reaction and biomedical application potential were discerned from these composites. DLS results showed that the zeta potential of pure ZnO NPs, Al-doped ZnO NPs, and Al-ZnO/rGO NCs were − 16.3 ± 8.30 mV, − 20.2 ± 6.86 mV, and 21.0 ± 14.10 mV, respectively. In a photocatalytic experiment, Al-ZnO/rGO nanocomposite showed enhanced degradation efficiency (82.49%) for Brilliant Blue R dye compared to pure ZnO (59.70%). Cytotoxicity evaluations against colorectal cancer (HCT116) cells showed markedly superior anticancer efficacy of Al-ZnO/rGO nanocomposites after both 24 and 48 h, higher than that of pure ZnO and Al-doped ZnO nanoparticles. The findings highlight the combined effect of aluminum doping and reduced graphene oxide incorporation to enhance the photocatalytic and anticancer efficacy of zinc oxide-based nanomaterials.

由于氧化锌纳米颗粒具有独特的可调物理化学性质,其在癌症治疗和光催化方面的应用受到了广泛的关注。本研究的新颖之处在于采用绿色方法,利用石榴皮提取物合成纯ZnO NPs、al掺杂ZnO NPs和Al-ZnO/rGO NCs,以提高其光催化和抗癌性能。通过XRD、SEM、EDX、XPS、FTIR、PL和DLS对合成材料进行了表征。XRD结果证实了ZnO的高结晶度,并表明掺杂和还原氧化石墨烯的掺入使ZnO的晶粒尺寸从17.60 nm增加到21.51 nm。ZnO纳米粒子在氧化石墨烯表面呈均匀分布的球形结构。EDX证实了纳米复合材料中存在Zn、O、Al和C,没有观察到杂质,而XPS则揭示了元素组成和氧化态。FTIR也支持官能团的存在,UV-Vis结果显示,由于掺杂和还原氧化石墨烯的集成,带隙能量从3.34 eV降低到3.25 eV。根据PL数据,推测这些复合材料具有更好的电荷分离性能,改善了光催化反应和生物医学应用潜力。DLS结果表明,纯ZnO NPs、al掺杂ZnO NPs和Al-ZnO/rGO NCs的zeta电位分别为- 16.3±8.30 mV、- 20.2±6.86 mV和21.0±14.10 mV。在光催化实验中,Al-ZnO/rGO纳米复合材料对Brilliant Blue R染料的降解效率(82.49%)高于纯ZnO(59.70%)。对结直肠癌(HCT116)细胞的细胞毒性评估显示,Al-ZnO/rGO纳米复合材料在24和48 h后的抗癌效果明显优于纯ZnO和al掺杂ZnO纳米颗粒。研究结果强调了铝掺杂和还原氧化石墨烯掺入的联合作用,以增强氧化锌基纳米材料的光催化和抗癌功效。
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引用次数: 0
Polymer-anchored vanadium(IV)–substituted benzimidazole: an Efficient green catalyst for aqueous oxidation of organic substrates 聚合物锚定钒(IV)取代苯并咪唑:有机底物水氧化的高效绿色催化剂
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-08 DOI: 10.1007/s11164-025-05809-9
M. L. Shilpa, B. Roopashree, V. Gayathri

Vanadium complexes are efficacious catalysts for the oxidation of diverse organic substrates. Immobilizing these complexes on solid supports enhances their chemical and thermal stability, improves catalytic efficiency, and facilitates easy separation from the reaction mixture, thereby minimizing contamination of the final product. A novel vanadium complex of substituted benzimidazole, 2(2'-quinolylbenzimodazole) immobilized on a partially chloromethylated polystyrene cross linked with divinyl benzene copolymer support was synthesized successfully. The supported catalyst was characterized by elemental analyses, TGA, conductivity and magnetic susceptibility measurements, FT-IR and Diffused Reflectance and Electron Spin Resonance spectral analysis. The proposed catalyst revealed positive outcomes in the oxidation reactions of Phenol, p-Nitrophenol, p-Cresol, Benzyl alcohol and p-Chlorobenzyl alcohol in water under ambient reaction conditions with H2O2 as an oxidant. The catalyst under ideal concentration and ambient reaction conditions exhibited excellent activity towards the green oxidation of Phenol with 99% conversion with 96% selectivity toward catechol at 60 °C. Similarly, p-nitrophenol exhibited a 95% conversion with 86% selectivity toward p-nitrocatechol. Additionally, the oxidation of p-cresol resulted in a 99% conversion and 92% selectivity toward p-hydroxybenzaldehyde. The catalyst also displayed excellent recyclability and facile separation, underscoring its potential for sustainable oxidation processes. It could be recycled for five turns retaining the catalytic activity of 92 to 94% with negligible leaching of only 0.25% of the embedded metal. The results suggested immobilized vanadium complex as an environmentally benign catalytic system to oxidize phenolic compounds in water.

钒配合物是多种有机底物氧化的有效催化剂。将这些配合物固定在固体载体上,增强了它们的化学和热稳定性,提高了催化效率,便于从反应混合物中分离,从而最大限度地减少了最终产物的污染。成功地合成了一种新型取代苯并咪唑- 2(2′-喹啉苯并咪唑)钒配合物,并将其固定在部分氯甲基化聚苯乙烯-二乙烯基苯交联共聚物载体上。通过元素分析、热重分析、电导率、磁化率、红外光谱、漫反射光谱和电子自旋共振光谱对负载催化剂进行了表征。该催化剂在常压条件下,以H2O2为氧化剂,对苯酚、对硝基苯酚、对甲酚、苯甲醇和对氯苯醇在水中的氧化反应均有良好的效果。在理想浓度和环境反应条件下,该催化剂对苯酚的绿色氧化活性优异,在60℃条件下,对邻苯二酚的转化率为99%,选择性为96%。同样,对硝基苯酚对对硝基儿茶酚的转化率为95%,选择性为86%。此外,对甲酚的氧化对对羟基苯甲醛的转化率为99%,选择性为92%。该催化剂还显示出优异的可回收性和易于分离性,强调了其可持续氧化过程的潜力。它可以循环使用5圈,保持92 - 94%的催化活性,浸出率仅为0.25%,可以忽略不计。结果表明,固定化钒配合物是一种环境友好的氧化水中酚类化合物的催化体系。
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引用次数: 0
Biocompatible manganese-tannic acid-βcyclodextrin compounds as catalytic antioxidants 生物相容性锰-单宁酸-β环糊精化合物作为催化抗氧化剂
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-07 DOI: 10.1007/s11164-025-05802-2
Mahtab Pirouzmand, Nardin Mosanaei Najibi, Saeedeh Khadivi-Derakhshan, Adel Mahmoudi Gharehbaba, Jafar Soleymani

In this study, a straightforward and eco-friendly approach was developed for the synthesis of biocompatible compounds that include manganese and tannic acid covalently linked with β-cyclodextrin (Mn/TA-βCD and MnTA/βCD). Additionally, a MnO2/TA-βCD composite was prepared for comparison. FT-IR, UV–vis, TGA, and Fluorescence techniques were used to characterize the prepared samples. TGA analysis demonstrated that MnTA/βCD had better thermal stability than Mn/TA-βCD. An interaction between β-cyclodextrin and tannic acid was confirmed by the fluorescence spectrum. The introduction of tannic acid into the β-cyclodextrin further improved the in vitro antioxidant potential. According to the pyrogallol autoxidation, MnTA/βCD exhibited the highest SOD-like activity (93%), and MnO2/TA-βCD demonstrated superior efficacy in scavenging hydrogen peroxide (94%). In addition, MTT assay studies confirmed the non-cytotoxic nature of the compounds.

在这项研究中,我们开发了一种简单、环保的方法来合成生物相容性化合物,包括锰和单宁酸与β-环糊精共价连接(Mn/TA-βCD和MnTA/βCD)。此外,制备了MnO2/TA-βCD复合材料进行比较。利用FT-IR、UV-vis、TGA和荧光技术对制备的样品进行表征。TGA分析表明MnTA/βCD比Mn/TA-βCD具有更好的热稳定性。荧光光谱证实了β-环糊精与单宁酸之间存在相互作用。单宁酸的引入进一步提高了β-环糊精的体外抗氧化能力。根据邻苯三酚的自氧化作用,MnTA/βCD表现出最高的sod样活性(93%),MnO2/TA-βCD表现出更强的过氧化氢清除能力(94%)。此外,MTT试验研究证实了化合物的非细胞毒性。
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引用次数: 0
Study on the preparation of cobalt catalyst and its catalytic reaction of diisobutene hydroesterification 钴催化剂的制备及其催化二异丁烯加氢酯化反应的研究
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-05 DOI: 10.1007/s11164-025-05795-y
Heyuan Song, Zhaoxiong Tian, Fanyu Zhao, Kunyao Zhang, Rui Ding, Daming Sun

The performance of graphitic carbon nitride (g-C3N4)-based cobalt (Co) catalysts (Co-g-C3N4, Co@g-C3N4) for the hydroesterification of diisobutylene (DIB) was evaluated. In this study, graphite carbon nitride (g-C3N4) was synthesized by that thermal decomposition of urea, melamine and thiourea in a muffle furnace. The results showed that the optimal reaction conditions were CO pressure 8.0 MPa, reaction temperature 150 °C and reaction time 10 h. When Co2(CO)8-g-C3N4 in situ catalyst was used, the conversion of DIB was 94.6% and the selectivity to methyl isononanoate was 90.0%. Similarly, in order to solve the problem of poor reusability of the catalyst, Co(OAc)2@g-C3N4 catalyst system prepared by impregnation method was studied. Under the same reaction conditions for 12 h, only 72.0% conversion of DIB and 89.6% selectivity to methyl isononanoate were obtained, but the catalytic performance was obviously improved compared with in situ catalyst. The catalysts were characterized by scanning electron microscope (SEM), Fourier transform infrared spectrometer (FT-IR), N2 adsorption–desorption isotherm and so on. In addition, the two catalyst systems are suitable for the hydroesterification reaction of various terminal olefins, and exhibit excellent recovery performance and thermal stability.

Graphical abstract

考察了石墨氮化碳(g-C3N4)基钴(Co)催化剂(Co-g-C3N4, Co@g-C3N4)在二异丁烯(DIB)加氢酯化反应中的性能。本研究以尿素、三聚氰胺和硫脲为原料,在马弗炉中热分解合成了石墨氮化碳(g-C3N4)。结果表明,最佳反应条件为CO压力8.0 MPa,反应温度150℃,反应时间10 h。采用Co2(CO)8-g-C3N4原位催化剂时,DIB的转化率为94.6%,异壬酸甲酯的选择性为90.0%。同样,为了解决催化剂重复使用性差的问题,对浸渍法制备的Co(OAc)2@g-C3N4催化剂体系进行了研究。在相同的反应条件下反应12 h, DIB的转化率仅为72.0%,异壬酸甲酯的选择性为89.6%,但催化性能较原位催化剂有明显提高。采用扫描电镜(SEM)、傅里叶变换红外光谱仪(FT-IR)、N2吸附-脱附等温线等对催化剂进行了表征。此外,两种催化剂体系均适用于多种末端烯烃的加氢酯化反应,并表现出优异的回收性能和热稳定性。图形抽象
{"title":"Study on the preparation of cobalt catalyst and its catalytic reaction of diisobutene hydroesterification","authors":"Heyuan Song,&nbsp;Zhaoxiong Tian,&nbsp;Fanyu Zhao,&nbsp;Kunyao Zhang,&nbsp;Rui Ding,&nbsp;Daming Sun","doi":"10.1007/s11164-025-05795-y","DOIUrl":"10.1007/s11164-025-05795-y","url":null,"abstract":"<div><p>The performance of graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>)-based cobalt (Co) catalysts (Co-g-C<sub>3</sub>N<sub>4</sub>, Co@g-C<sub>3</sub>N<sub>4</sub>) for the hydroesterification of diisobutylene (DIB) was evaluated. In this study, graphite carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) was synthesized by that thermal decomposition of urea, melamine and thiourea in a muffle furnace. The results showed that the optimal reaction conditions were CO pressure 8.0 MPa, reaction temperature 150 °C and reaction time 10 h. When Co<sub>2</sub>(CO)<sub>8</sub>-g-C<sub>3</sub>N<sub>4</sub> in situ catalyst was used, the conversion of DIB was 94.6% and the selectivity to methyl isononanoate was 90.0%. Similarly, in order to solve the problem of poor reusability of the catalyst, Co(OAc)<sub>2</sub>@g-C<sub>3</sub>N<sub>4</sub> catalyst system prepared by impregnation method was studied. Under the same reaction conditions for 12 h, only 72.0% conversion of DIB and 89.6% selectivity to methyl isononanoate were obtained, but the catalytic performance was obviously improved compared with in situ catalyst. The catalysts were characterized by scanning electron microscope (SEM), Fourier transform infrared spectrometer (FT-IR), N<sub>2</sub> adsorption–desorption isotherm and so on. In addition, the two catalyst systems are suitable for the hydroesterification reaction of various terminal olefins, and exhibit excellent recovery performance and thermal stability.</p><h3>Graphical abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"52 1","pages":"263 - 285"},"PeriodicalIF":3.5,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145904486","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
An efficient and environmentally benign nanocatalytic approach for the one-pot, multicomponent synthesis of 1,3-thiazolidin-4-ones 一种高效、环保的一锅多组分合成1,3-噻唑烷-4-酮的纳米催化方法
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-05 DOI: 10.1007/s11164-025-05808-w
Datta M. Gumatkar, Shraddha V. Jadhav, Navnath T. Hatvate, Yatin U. Gadkari

A mild and robust synthetic strategy has been developed for the synthesis of 1,3-thiazolidin-4-one derivatives via a one-pot, three-component reaction of aromatic or heteroaromatic aldehydes, aromatic amines, and thioglycolic acid under solvent-free conditions at 110 °C. The reaction proceeds efficiently in the presence of iron oxide nanoparticles coated with hydroxyapatite (Fe3O4/HAP), serving as a heterogeneous solid-base nanocatalyst. This nanocatalyst produces good to excellent yields desired product and offers several practical advantages. Comprehensive characterization of the catalyst was performed using X-ray diffraction, Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), and field emission scanning electron microscopy. The new synthetic methodology has a shorter reaction time, a broad-substrate scope, and an eco-friendly and solvent-free approach. Due to its strong magnetic responsiveness, the catalyst can be conveniently recovered using an external magnetic field and reused for five successive cycles with negligible loss in activity.

Graphical abstract

在110°C无溶剂条件下,通过芳香或杂芳香醛、芳香胺和巯基乙酸的一锅三组分反应,建立了一种温和而稳健的合成策略,用于合成1,3-噻唑烷-4-酮衍生物。在羟基磷灰石(Fe3O4/HAP)包裹的氧化铁纳米颗粒作为非均相固体基纳米催化剂存在下,反应有效进行。这种纳米催化剂可以产生良好到优异的收率,并具有一些实用的优点。采用x射线衍射、傅里叶红外光谱(FTIR)、热重分析(TGA)和场发射扫描电镜对催化剂进行了全面表征。新的合成方法具有反应时间短、底物范围广、环境友好、无溶剂等优点。由于催化剂具有较强的磁响应性,因此可以利用外磁场方便地回收,并且可以连续重复使用5次,而活性损失可以忽略不计。图形抽象
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引用次数: 0
Boosting photocatalytic activity of g-C3N4 via dual modification: protonation-induced exfoliation and NCDs-mediated charge separation 通过质子诱导的剥离和ncds介导的电荷分离双重修饰提高g-C3N4的光催化活性
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-05 DOI: 10.1007/s11164-025-05807-x
Gang Wang, Lan Yang, Yanning Yang, Zhiqiang Wu, Jing Wang, Yongyan Ye

A metal-free P-(g-C3N4/NCDs) photocatalytic composite was synthesized by modifying graphitic carbon nitride (g-C3N4) through a dual strategy of nitrogen-doped carbon quantum dots (NCDs) incorporation and protonation. Under light irradiation, the optimized catalyst achieved 99% degradation of methyl orange within 120 min, exhibiting a reaction rate 50 times higher than that of unmodified g-C3N4. Furthermore, the composite demonstrated excellent stability, maintaining high catalytic performance over five consecutive cycles. Characterization results revealed that the dual modification induced a stripping effect on the g-C3N4 material. This process optimized the electronic structure of the composite, effectively suppressing the recombination of photogenerated electron–hole pairs. Additionally, adjustment of the band gap structure enhanced the oxidizing capacity of the valence band, thereby improving the overall photocatalytic activity. The synergistic effect of superoxide (•O2) and hydroxyl (•OH) radicals in substantially boosting the oxidative capacity of P-(g-C3N4/NCDs) was unambiguously verified by radical trapping experiments and electron paramagnetic resonance (EPR) spectroscopy. This synergy facilitates the mineralization of organic dye molecules into small inorganic molecules (e.g., CO2 and H2O). This metal-free photocatalyst design strategy, focused on material structure optimization, circumvents secondary water pollution from metal leaching, suggesting promising potential for applications in green catalysis and related fields.

通过氮掺杂碳量子点(NCDs)掺入和质子化的双重策略,对石墨氮化碳(g-C3N4)进行改性,合成了无金属P-(g-C3N4/NCDs)光催化复合材料。在光照下,优化后的催化剂在120 min内对甲基橙的降解率达到99%,反应速率比未改性的g-C3N4高50倍。此外,该复合材料表现出优异的稳定性,在连续五个循环中保持较高的催化性能。表征结果表明,双改性对g-C3N4材料产生了剥离效应。该工艺优化了复合材料的电子结构,有效抑制了光生电子-空穴对的复合。此外,带隙结构的调整增强了价带的氧化能力,从而提高了整体光催化活性。超氧自由基(•O2−)和羟基自由基(•OH)在显著提高P-(g-C3N4/NCDs)氧化能力方面的协同作用得到了自由基捕获实验和电子顺磁共振(EPR)光谱的明确证实。这种协同作用有助于有机染料分子矿化成小的无机分子(例如CO2和H2O)。这种以优化材料结构为重点的无金属光催化剂设计策略,避免了金属浸出对水体的二次污染,在绿色催化及相关领域具有广阔的应用前景。
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引用次数: 0
Formation of active bimetallic species in Pd–Mn/Sibunit catalysts for selective hydrogenation of acetylene to ethylene Pd-Mn / siunit催化剂中乙炔选择性加氢制乙烯活性双金属的形成
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-04 DOI: 10.1007/s11164-025-05804-0
Daria V. Yurpalova, Zakhar S. Vinokurov, Evgeny V. Khramov, Igor P. Prosvirin, Maxim A. Panafidin, Andrey V. Bukhtiyarov, Evgeny Yu. Gerasimov, Mikhail V. Trenikhin, Larisa M. Kovtunova, Vyacheslav L. Yurpalov

New bimetallic Pd–Mn catalysts supported on the carbon material Sibunit have been obtained and studied for the process of producing ethylene by acetylene hydrogenation. The composition, structure, morphology and electronic state of the active phase have been studied in detail depending on the temperature of treatment in hydrogen and the Pd/Mn ratio by XRD, XANES, EXAFS, TEM, XPS. It has been found that the active species are the nanoparticles of intermetallic tetragonal structure Pd3Mn2 that formed during the treatment of Pd–Mn/Sibunit in H2 at 500 °C. Increasing the reduction temperature to 600–700 °C provides an increase in the proportion of the Pd3Mn2 phase due to more complete involvement of palladium in the interaction with manganese. Pd3Mn2 nanoparticles are less active but more selective than Pd nanoparticles due to changes in the geometry of active sites and their electronic state. It is shown that catalysts containing a twofold molar excess of Mn relative to Pd are characterized by the presence of more dispersed bimetallic particles than samples containing less manganese, due to which they are characterized by higher activity. Pd–Mn/Sibunit catalysts provide a high ethylene yield (up to 75%), which makes them promising materials for the process of acetylene hydrogenation to ethylene.

Graphical abstract

研究了以硅基为载体的新型双金属钯锰催化剂在乙炔加氢制乙烯工艺中的应用。利用XRD、XANES、EXAFS、TEM、XPS等分析手段对不同处理温度下活性相的组成、结构、形貌和电子态进行了详细的研究。结果表明,活性物质为500℃下Pd-Mn /Sibunit在H2中处理形成的金属间四方结构的Pd3Mn2纳米粒子。将还原温度提高到600-700°C,由于钯与锰的相互作用更完全地参与,Pd3Mn2相的比例增加。由于活性位点的几何形状和电子状态的改变,Pd3Mn2纳米粒子比Pd纳米粒子活性更低,但选择性更强。结果表明,与锰含量较低的样品相比,锰含量为Pd的两倍摩尔过量的催化剂具有更分散的双金属颗粒,因此具有更高的活性。Pd-Mn /Sibunit催化剂具有较高的乙烯产率(高达75%),是乙炔加氢制乙烯的理想材料。图形抽象
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引用次数: 0
CeVO4 materials prepared by a coprecipitation approach as non-noble metal oxide catalysts for liquid-phase aerobic oxidation of benzyl alcohol by atmospheric O2 用共沉淀法制备CeVO4材料作为常压O2液相好氧氧化苯甲醇的非贵金属氧化物催化剂
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-03 DOI: 10.1007/s11164-025-05805-z
Ru-Meng Yu, Ya-Qi Miao, Rui-Min Wang, Fei Wang, Jie Xu, Bing Xue

Liquid-phase selective oxidation of benzyl alcohol (BZA) by atmospheric O2 is a sustainable route for the synthesis of benzaldehyde (BZL). Although noble metal catalysts showed excellent activity, the high cost and limited reserves of noble metals underscore the significance of developing efficient non-noble metal-based catalysts. Herein, cerium vanadate (CeVO4) materials were synthesized by a simple coprecipitation method and employed as heterogeneous catalysts for the selective oxidation of BZA by O2. Under the same reaction conditions, the CeVO4 materials demonstrated superior activity to the pure V2O5 and CeO2 samples, affording a high yield of BZL of 69% under a reaction temperature of 120 °C. For the CeVO4 materials, the catalytic activity correlated well with the percentages of Ce3+ and V4+ species, depending on the preparation temperatures. Moreover, the catalysts could be reused at least five times without significant loss in activity.

Graphical abstract

常压O2液相选择性氧化苯甲醇(BZA)是合成苯甲醛(BZL)的可持续途径。虽然贵金属催化剂表现出优异的活性,但昂贵的成本和有限的贵金属储量凸显了开发高效的非贵金属催化剂的重要性。本文采用简单共沉淀法合成了钒酸铈(CeVO4)材料,并将其作为O2选择性氧化BZA的多相催化剂。在相同的反应条件下,CeVO4材料表现出优于纯V2O5和CeO2样品的活性,在120℃的反应温度下,BZL的产率高达69%。对于CeVO4材料,其催化活性与Ce3+和V4+的含量相关,且与制备温度有关。此外,催化剂可以重复使用至少五次而不会有明显的活性损失。图形抽象
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引用次数: 0
Enhanced photocatalytic performance of mixed-phase TiO2–RGO nanocomposite for fast methylene blue decomposition under visible light TiO2-RGO纳米复合材料在可见光下快速分解亚甲基蓝的光催化性能增强
IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-03 DOI: 10.1007/s11164-025-05799-8
Reza Naderzadeh, Masoud Vesali-Naseh, Majid Rezaeivala

Methylene blue (MB) as a persistent dye poses serious environmental threats, requiring efficient removal methods. In this study, the TiO2-graphene nanocomposites have been fabricated for MB decomposition under visible-light irradiation. Graphene oxide was synthesized via a modified Hummers method and subsequently incorporated into mixed-phase TiO2 (44% anatase and 56% rutile) in varying amounts (5–75 wt. %) using a hydrothermal method. The introduction of this oxygen-functionalized reduced graphene oxide (RGO) into the TiO2 matrix significantly enhanced the photocatalytic activity by increasing the adsorption surface area, reducing the band gap, and suppressing electron–hole recombination.

The nanocomposite with an optimal 50 wt. % RGO content demonstrated nearly complete MB degradation in less than 10 min, fitting a pseudo-first-order kinetic model with a high-rate constant. These results highlight the potential of TiO2–RGO nanocomposites for effective and rapid dye removal, presenting a promising advance in environmental remediation technologies.

亚甲基蓝作为一种持久性染料,对环境造成了严重的威胁,需要有效的去除方法。在本研究中,制备了二氧化钛-石墨烯纳米复合材料,在可见光照射下分解MB。通过改进的Hummers方法合成氧化石墨烯,随后使用水热法将不同量(5-75 wt. %)的混合TiO2(44%锐钛矿和56%金红石)掺入。将这种氧功能化的还原氧化石墨烯(RGO)引入TiO2基体中,通过增加吸附表面积、减小带隙和抑制电子-空穴复合,显著增强了TiO2的光催化活性。最佳RGO含量为50 wt. %的纳米复合材料在不到10分钟的时间内几乎完全降解了MB,符合高速率常数的准一级动力学模型。这些结果突出了二氧化钛-还原氧化石墨烯纳米复合材料在有效和快速去除染料方面的潜力,为环境修复技术提供了一个有希望的进展。
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Research on Chemical Intermediates
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