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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 Epub Date: 2024-03-08 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
Synthesis, properties, and utilization of carbon quantum dots as photocatalysts on degradation of organic dyes: A mini review 作为光催化剂降解有机染料的碳量子点的合成、特性和利用:微型综述
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-03-26 DOI: 10.1016/j.catcom.2024.106914
A. Muhammad Afdhal Saputra , Averroes Fazlur Rahman Piliang , Dellyansyah , Marpongahtun , Andriayani , Ronn Goei , Risky Ramadhan H.T.S. , Saharman Gea

This review highlights Carbon Quantum Dots (CQDs) as promising photocatalysts for breaking down organic pollutants, particularly in advancing CQDs-based systems for degrading organic dyes. CQDs, used alone or combined with semiconductors, enhance performance. In scenarios with narrow bandgaps, CQDs assist in separating charges, whereas in wider bandgaps, they enable visible/NIR activity through up-conversion luminescence. When integrated into Z-scheme heterostructures, CQDs reduce recombination by facilitating electron transfer. Synthesis methods—both top-down and bottom-up—are explored along with crucial physicochemical properties. Furthermore, modifying CQDs through doping and integrating functional groups on their surface adjusts their characteristics, promising more effective CQDs-modified photocatalysts in future research.

本综述重点介绍碳量子点(CQDs)作为分解有机污染物的光催化剂的前景,尤其是在推进基于 CQDs 的有机染料降解系统方面。CQDs 可单独使用,也可与半导体结合使用,从而提高性能。在带隙较窄的情况下,CQDs 可以帮助分离电荷;而在带隙较宽的情况下,它们可以通过上转换发光实现可见/近红外活性。当 CQDs 集成到 Z 型异质结构中时,可通过促进电子转移来减少重组。我们探讨了自上而下和自下而上的合成方法以及关键的物理化学特性。此外,通过在 CQDs 表面掺杂和整合功能基团来修饰 CQDs 可调整其特性,从而有望在未来的研究中获得更有效的 CQDs 修饰光催化剂。
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引用次数: 0
MOF-derived Fe3O4@SiO2/Al2O3 yolk-shell nanoreactor for efficient furfural acetalization 用于高效糠醛缩醛化的 MOF 衍生 Fe3O4@SiO2/Al2O3 卵黄壳纳米反应器
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-03-07 DOI: 10.1016/j.catcom.2024.106900
Yang Zhang , Qizhuang Zou , Ruiqi Fang , Hua Tan , Hongbing Ji , Yingwei Li

Yolk-shell nanoreactors feature numbers of advantages in promoting catalytic performance. This work demonstrates the fabrication of yolk-shell Fe3O4@SiO2/Al2O3-T (T = 500–900 °C) from metal-organic framework. Characterizations indicate the Fe3O4 yolk and SiO2/Al2O3 shell of the obtained nanoreactors. Fe3O4@SiO2/Al2O3–800 showed excellent performance in furfural acetalization to 2-(dimethoxymethyl)furan, achieving a 97% yield at 60 °C, atmospheric pressure within 5 h. Control experiments reveal the high reactivity of Fe3O4 yolks for furfural acetalization, and acidic Al species are favorable for reactivity promotion. Besides, porous SiO2/Al2O3 shells facilitate mass transfer and increase the accessibility of active sites, also contribute to the high performance and stability.

卵壳纳米反应器在提高催化性能方面具有诸多优势。这项工作展示了利用金属有机框架制备卵黄壳 Fe3O4@SiO2/Al2O3-T(T = 500-900℃)的过程。表征结果表明,获得的纳米反应器具有 Fe3O4 卵黄和 SiO2/Al2O3 外壳。对照实验结果表明,Fe3O4@SiO2/Al2O3-800 在糠醛缩醛生成 2-(二甲氧基甲基)呋喃的过程中表现出优异的性能,在 60 ℃、常压条件下,5 h 内的产率达到 97%。此外,多孔的 SiO2/Al2O3 壳有利于传质,增加了活性位点的可及性,也有助于提高性能和稳定性。
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引用次数: 0
An insight into the catalytic properties and process optimization of Fe, Ni doped eggshell derived CaO for a green biodiesel synthesis from waste chicken fat 深入了解掺杂铁、镍的蛋壳衍生氧化钙在利用废弃鸡脂肪合成绿色生物柴油过程中的催化特性和工艺优化
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.2024.106848
Rabiah Amal , Ruba Nadeem , Azeem Intisar , Hifza Rouf , Dilawar Hussain , Rehana Kousar

The basic theme of the current research work is based on the utilization of waste materials to produce environmentally friendly energy, i.e., waste + waste = energy. Efficacious and recyclable eggshell derived CaO, and transition metal doped CaO i.e. Fe-CaO, and Ni-CaO catalysts were used to synthesize biodiesel from chicken fat as a potential source of bioenergy. The synthesized catalysts were examined using a variety of analysis methods, such as FTIR, SEM, and XRD. Single step transesterification process gave 83% biodiesel yield using Fe-CaO. The characteristics of synthesized biodiesel were compared with international standards (ASTM6751 and EU14214).

当前研究工作的基本主题是利用废料生产环保能源,即废物+废物=能源。研究人员利用高效且可回收的蛋壳衍生 CaO 和过渡金属掺杂 CaO(即 Fe-CaO 和 Ni-CaO 催化剂)从鸡脂肪中合成生物柴油,以此作为一种潜在的生物能源。使用傅立叶变换红外光谱、扫描电镜和 X 射线衍射等多种分析方法对合成的催化剂进行了检测。使用 Fe-CaO 进行的单步酯交换反应产生了 83% 的生物柴油。合成生物柴油的特性与国际标准(ASTM6751 和 EU14214)进行了比较。
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引用次数: 0
Enhanced electrocatalytic HER performances of metal free SiC/g-C3N5 heterostructures 增强无金属 SiC/g-C3N5 异质结构的电催化 HER 性能
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-02-20 DOI: 10.1016/j.catcom.2024.106882
Sethumathavan Vadivel , P. Sujita , Bappi Paul , B. Vidhya , Anju Sebastian , R. Selvarajan

Here in, we have fabricated a composite of SiC and g-C3N5 to form a noble-metal-free heterostructure as SiC/g-C3N5 for electrochemical HER activity. More than a few characterization techniques were investigated for their structural properties, such as the XRD, UV- DRS, FT-IR, FE-SEM, HR-TEM, and XPS measurements respectively. The HER reaction of SiC/g-C3N5 heterostructure with an overpotential obtained from Tafel slope of 81 mV/dec vs RHE at 10 mA/cm2 which is much better than that of the pristine SiC material. This work entitles that the effective approach for the rational design of g-C3N5-based electrocatalysts, for future developments in metal-free electrocatalysts.

在此,我们制备了 SiC 和 g-C3N5 的复合材料,形成了一种不含惰性金属的异质结构 SiC/g-C3N5,用于电化学 HER 活性。研究人员采用了多种表征技术,如 XRD、UV- DRS、FT-IR、FE-SEM、HR-TEM 和 XPS 测量等,对其结构特性进行了研究。在 10 mA/cm2 的条件下,SiC/g-C3N5 异质结构的 HER 反应的过电位为 81 mV/dec vs RHE,远高于原始 SiC 材料的过电位。这项工作为合理设计基于 g-C3N5 的电催化剂提供了有效方法,有助于未来无金属电催化剂的发展。
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引用次数: 0
AgNi/PC bimetallic and AgNi/PC@Mn trimetallic nanocatalysts for the efficient reduction of 4-nitrophenol 用于高效还原 4-硝基苯酚的 AgNi/PC 双金属和 AgNi/PC@Mn 三金属纳米催化剂
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-02-23 DOI: 10.1016/j.catcom.2024.106885
Hikmet Beyza Erdem, Sevil Çetinkaya

Catalytic efficiency in hydrogenation reactions can be increased due to the stability achieved with nanomaterials prepared by homogeneously immobilizing multiple metal nanoparticles onto porous solid materials. Herein, porous carbon (PC)-supported bimetallic (AgNi/PC) and trimetallic nanoparticles (AgNi/PC@Mn) were developed and evaluated as catalysts in the NaBH4-mediated reduction of 4-nitrophenol to 4-aminophenol. AgNi/PC@Mn catalysts were synthesized using a two-step synthesis strategy. The highest and excellent catalytic efficiency under ambient conditions was obtained by the trimetallic catalyst. Both catalysts proved to be easily separated from the reaction medium and usable for up to five consecutive cycles without losing their catalytic activity.

通过将多种金属纳米颗粒均匀固定在多孔固体材料上制备的纳米材料具有稳定性,可以提高加氢反应的催化效率。本文开发了多孔碳(PC)支撑的双金属(AgNi/PC)和三金属纳米颗粒(AgNi/PC@Mn),并将其作为 NaBH4 介导的 4-硝基苯酚还原为 4-氨基苯酚的催化剂进行了评估。AgNi/PC@Mn 催化剂采用两步合成策略合成。在环境条件下,三金属催化剂的催化效率最高且性能优异。事实证明,这两种催化剂都很容易从反应介质中分离出来,并可连续使用五个循环而不会失去催化活性。
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引用次数: 0
Photocatalytic CO2 reduction coupled with biomass-based amines oxidation over double-shelled CdS nanocages 双壳 CdS 纳米笼光催化二氧化碳还原和生物胺氧化
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-02-23 DOI: 10.1016/j.catcom.2024.106884
Haoran Liu , Hanlin Zhou , Luowen Yang , Yixian Pan , Xin Zhao , Fengliang Wang , Ruiqi Fang , Yingwei Li

Solar-driven CO2 reduction to CO production is often hampered by the kinetically sluggish water photooxidation and fast recombination of photocarriers. Herein, we report a photoredox system of CO2 reduction coupled with biomass-based amines oxidation. Double-shelled CdS nanocages (CdS DSNC) are synthesized by a successive etching‑sulfuration strategy, which delivers impressive CO and difurfurylamine yields of 1226.4 and 5526.5 μmol·g−1·h−1, respectively. Mechanism studies uncover that the double-shelled structure endows CdS DSNC with high accessibility of active sites and short transfer distance for photocarriers. Besides, furfurylamine serves as both the electron donor and the capturer of CO2, thus boosting the photoredox performance.

太阳能驱动的二氧化碳还原生成一氧化碳的过程往往受到动力学缓慢的水光氧化作用和光载体快速重组的阻碍。在此,我们报告了一种二氧化碳还原与生物质胺氧化耦合的光氧化系统。通过连续刻蚀-硫化策略合成了双壳 CdS 纳米笼(CdS DSNC),其 CO 和二糠胺产率分别达到了惊人的 1226.4 μmol-g-1-h-1 和 5526.5 μmol-g-1-h-1。机理研究发现,双壳结构使 CdS DSNC 具有高活性位点可达性和光载体传输距离短的特点。此外,糠胺既是电子供体,又是二氧化碳的捕获体,从而提高了光氧化性能。
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引用次数: 0
Cycloalkanes oxidation with O2 catalyzed by a novel metalloporphyrin-based covalent coupling structure with bimetallic catalytic centers through synergistic mode 基于金属卟啉的新型共价偶联结构与双金属催化中心通过协同模式催化环烷烃与 O2 的氧化反应
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-02-13 DOI: 10.1016/j.catcom.2024.106876
Jia-Ye Ni, Yan-Bo Ding, Jing Sun, Hong-Ke Wu, Hai-Min Shen, Yuan-Bin She

A novel bimetallic central covalent coupling catalytic system (Porp.Co@Zn-C6) based on Tris(4-Cl)(4-OH)Co and Tris(4-Cl)(4-OH)Zn was established to improve cycloalkanes oxidation. In particular, the partially-oxidized product's selectivity rose from 86.4% to 97.5% and the cyclohexane conversion was boosted from 3.80% to 4.41%. Simultaneously achieved improvements in conversion and selectivity. In this system, Co(II) was employed to activate molecular oxygen, Zn(II) was utilized to strengthen the utilization of cyclohexyl hydroperoxide and to be avoided its thermal decomposition in disorder state. This proposal can be very suitable for other cycloalkanes as well, which will improve the conversion and selectivity concurrently.

建立了一种基于三(4-Cl)(4-OH)Co 和三(4-Cl)(4-OH)Zn 的新型双金属中心共价偶联催化体系 (Porp.Co@Zn-C6),以改善环烷烃的氧化。其中,部分氧化产物的选择性从 86.4% 提高到 97.5%,环己烷的转化率从 3.80% 提高到 4.41%。同时提高了转化率和选择性。在该系统中,Co(II) 被用来激活分子氧,Zn(II) 被用来加强环己基过氧化氢的利用,并避免其在无序状态下的热分解。这一建议也非常适用于其他环烷烃,可同时提高转化率和选择性。
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引用次数: 0
DoE-driven thermodynamic assessment of COX-free hydrogen production from methane decomposition 由 DoE 驱动的甲烷分解无 COX 制氢热力学评估
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.2024.106874
Lucas David Biondo , Christian Manera , Cesar Aguzzoli , Marcelo Godinho

Methane decomposition for hydrogen production is classified as blue turquoise, an intermediate between green and blue hydrogen. It does not generate greenhouse gas (GHG) emissions and does not require installation of carbon capture, utilization, and storage (CCUS) processes, becoming environmentally competitive among technologies, as the only byproduct is solid carbon. This research contributes to optimize temperature and gas hourly space velocity parameters for methane conversion adopting design of experiment (DoE) concept to collect data and identify significant factors through a 32 factorial design. Highest methane conversion, considering thermodynamic equilibrium limit of reaction, was obtained at 900 K and 6000 mL.h−1.g−1. The catalyst used was characterized by SEM, BET, and XRD.

甲烷分解制氢被归类为蓝色绿松石,介于绿色和蓝色氢气之间。它不会产生温室气体(GHG)排放,也不需要安装碳捕获、利用和储存(CCUS)工艺,在各种技术中具有环境竞争力,因为唯一的副产品是固体碳。本研究采用实验设计(DoE)概念,通过 32 因子设计收集数据并确定重要因素,从而优化甲烷转化的温度和气体小时空间速度参数。考虑到反应的热力学平衡极限,在 900 K 和 6000 mL.h-1.g-1 条件下获得了最高的甲烷转化率。使用的催化剂通过 SEM、BET 和 XRD 进行了表征。
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引用次数: 0
Influence of binder selection on the catalytic performance of zeolite-based bifunctional catalysts for biomass catalysis 粘合剂选择对生物质催化用沸石基双功能催化剂催化性能的影响
IF 3.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 Epub Date: 2024-03-02 DOI: 10.1016/j.catcom.2024.106892
Jinfei Lu , Shaohua Wang , Yanheng Hao , Lu Lin , Fan Bai , Wenhao Cui , Juan Wang , Qingda An , Peng Tian , Jifeng Pang , Wenhao Luo

The impact of binder selection on catalytic performance of real catalyst extrudates is still limitedly shown in biomass catalysis. Herein, we have prepared two zeolite-based bifunctional extrudates (Ni/LaY-Al2O3 and Ni/LaY-SiO2). Compared with Ni/LaY-Al2O3, Ni/LaY-SiO2 shows a markedly enhanced durability and sustained performance for 936 h in the continuous liquid-phase hydrogenation of γ-valerolactone into methyl pentanoate. Complementary characterization studies reveal that choosing SiO2 as binder could efficiently mitigate metal agglomeration, coke formation and support dealumination during catalysis. These findings showcase that binder selection is essential for catalyst durability in the development of the industrial-level bifunctional catalysts for biomass valorization.

在生物质催化领域,粘合剂的选择对实际催化剂挤出物催化性能的影响还很有限。在此,我们制备了两种基于沸石的双功能挤出物(Ni/LaY-AlO 和 Ni/LaY-SiO)。与 Ni/LaY-AlO 相比,Ni/LaY-SiO 在将γ-戊内酯连续液相氢化为戊酸甲酯的过程中显示出明显更强的耐久性和持续 936 小时的性能。补充性表征研究表明,选择氧化硅作为粘合剂可有效缓解催化过程中的金属团聚、焦炭形成和支撑脱气。这些研究结果表明,在开发用于生物质资源化的工业级双功能催化剂时,粘合剂的选择对催化剂的耐久性至关重要。
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引用次数: 0
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Catalysis Communications
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