Molecular Catalysis最新文献_第10页

Nickel nanoparticles embedded in N-doped carbon efficient selective hydrogenation of cinnamaldehyde in aqueous phase 纳米镍包埋在n掺杂碳中，肉桂醛在水相中高效选择性加氢

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-19 DOI: 10.1016/j.mcat.2025.115608

Xingguo Yang , Xinhuan Lu , Qinjun Zhang , Hao Liu , Haotian Guo , Lin Zhao , Dan Zhou , Qinghua Xia

The selective hydrogenation of cinnamaldehyde (CAL) to cinnamyl alcohol (COL) is challenging because the hydrogenation of C = C bonds is thermodynamically favored over that of the C = O group. In this work, Ni₃/Fe@CN-x materials prepared by loading metal Ni onto carbon materials derived from Fe-ZIF were successfully used to selectively hydrogenate the C = O bond of cinnamaldehyde, while single metal Ni@CN-x materials derived from Ni-ZIF materials were successfully used to selectively hydrogenate the C = C bond in the side chain of CAL. Both catalysts shows admirable catalytic activity in the selective hydrogenation reaction of CAL. The reaction results show that the introduction of Ni species into Fe@CN-350 material significantly improved the conversion of CAL and the selectivity of COL, which is attributed to the synergistic effect of bimetallic Ni and Fe, and the excellent hydrogenation activity of metallic Ni. The Ni₃/Fe@CN-350 catalytic system can achieved 94.3 % CAL conversion and 86.3 % COL selectivity, and the catalyst could be stably recycled 5 times. Under mild conditions (90 °C, 4 h), the single metal Ni@CN-600 catalytic system achieved 100 % CAL conversion and >99 % hydrocinnamaldehyde (HCAL) selectivity, and the catalyst could be stably recycled 10 times.

肉桂醛（CAL）选择性氢化成肉桂醇（COL）是具有挑战性的，因为C = C键的氢化在热力学上比C = O基团的氢化更有利。在这项工作中，通过将金属Ni加载到Fe-ZIF衍生的碳材料上制备的Ni3/Fe@CN-x材料成功地用于选择性氢化肉桂醛的C = O键。而由Ni- zif材料衍生的单金属Ni@CN-x材料则成功地对CAL侧链上的C = C键进行了选择性加氢。两种催化剂在CAL的选择性加氢反应中都表现出了良好的催化活性。反应结果表明，在Fe@CN-350材料中引入Ni物种显著提高了CAL的转化率和COL的选择性，这归因于双金属Ni和Fe的协同作用。金属Ni具有优异的加氢活性。Ni3/Fe@CN-350催化体系CAL转化率为94.3%，COL选择性为86.3%，催化剂可稳定循环使用5次。在温和条件下（90℃，4 h），单金属Ni@CN-600催化体系实现了100%的CAL转化率和>； 99%的氢肉桂醛（HCAL）选择性，催化剂可稳定循环10次。

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引用次数: 0

Understanding nanogel–MOF synergism in the stabilization of Candida rugosa lipase: A molecular dynamics simulation study 了解纳米凝胶- mof在稳定念珠菌脂肪酶中的协同作用：分子动力学模拟研究

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-19 DOI: 10.1016/j.mcat.2025.115607

Prasanna J. Patil , Xin Liang , Hassan bin Waseem , Subodh A. Kamble , Nagesh Manurkar , Akhtiar Ali , Haroon Shah , Weiwei Li , Xiuting Li

The catalytic performance and structural stability of Candida rugosa lipase (CRL) often deteriorate under harsh reaction conditions such as high temperature, extreme pH, or organic solvents, limiting its industrial applicability. Enzyme immobilization has emerged as a promising strategy to overcome these challenges, with nanogels and metal–organic frameworks (MOFs) among the most effective supports. In this study, molecular dynamics (MD) simulations were employed to investigate the cooperative stabilization effects of acrylamide-based nanogels and the representative MOF ZIF-8 on CRL. Building upon our previous experimental and computational work, this is the first study to elucidate, at the atomistic level, the molecular mechanisms governing enzyme stabilization within a hybrid nanogel–MOF confinement. The investigation was performed in two stages: (i) analysis of the self-assembly and conformational stability of the CRL–nanogel complex and (ii) evaluation of its interaction with ZIF-8 compared to the free CRL–ZIF-8 system. The results demonstrate that nanogel confinement significantly reduces conformational fluctuations [average root mean square deviation (RMSD) ≈ 0.23 nm vs. 0.36 nm in free CRL–ZIF-8], increases hydrogen-bond formation by ∼20 %, and decreases solvent-accessible surface area (SASA) by ∼15 %, thereby maintaining active-site geometry and overall structural integrity. These findings provide the first molecular-level evidence of nanogel–MOF synergism in enzyme stabilization and establish a framework for designing next-generation hybrid immobilization platforms that integrate flexibility, hydration, and rigidity to enhance biocatalytic performance.

念珠菌脂肪酶（Candida rugosa lipase， CRL）在高温、极端pH或有机溶剂等恶劣反应条件下，其催化性能和结构稳定性经常恶化，限制了其工业应用。酶固定化已成为克服这些挑战的一种有前途的策略，纳米凝胶和金属有机框架（mof）是最有效的支持。本研究采用分子动力学（MD）模拟研究了丙烯酰胺基纳米凝胶与具有代表性的MOF ZIF-8对CRL的协同稳定作用。在我们之前的实验和计算工作的基础上，这是第一个在原子水平上阐明在混合纳米凝胶- mof约束下控制酶稳定的分子机制的研究。研究分两个阶段进行：(i)分析crl -纳米凝胶复合物的自组装和构象稳定性；（ii）与游离的CRL-ZIF-8体系相比，评估其与ZIF-8的相互作用。结果表明，纳米凝胶约束显著降低构象波动[平均均方根偏差(RMSD)≈0.23 nm vs.游离cr - zif -8的0.36 nm]，增加氢键形成约20%，减少溶剂可及表面积（SASA）约15%，从而保持活性位点的几何形状和整体结构完整性。这些发现为纳米凝胶- mof在酶稳定中的协同作用提供了第一个分子水平的证据，并为设计下一代混合固定化平台建立了框架，该平台集成了柔韧性、水合性和刚性，以提高生物催化性能。

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引用次数: 0

Regulation of β-ketoenamine COFs planarity for enhanced photocatalytic oxidation/dehydrogenation performance 调节β-酮胺COFs平面度以增强光催化氧化/脱氢性能

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-19 DOI: 10.1016/j.mcat.2025.115603

Xiaojie Wu , Shibing Wu , Run Wang , Mingyue Chen , Jiang Liu , Xilong Yan , Yang Li , Bowei Wang , Ligong Chen

The planarity of covalent organic frameworks (COFs) is a critical structural parameter for their photocatalytic performance. However, its influence on the efficiency of photocatalytic organic transformations has not been fully investigated. Herein, three β-ketoenamine COFs with different planarity, denoted as TP-EDDA-COF, TP-DATP-COF, and TP-DMTP-COF, were synthesized to explore the influence of planarity on their photocatalytic performance. With the best planarity, TP-EDDA-COF exhibited a superior visible-light absorption range and photogenerated carrier separation and migration efficiency. Therefore, it demonstrated exceptional photocatalytic performance, with conversions reaching 98 % for the dehydrogenation of tetrahydroquinoline (THQ) and 99 % for the oxidative coupling of benzylamine (BA). Furthermore, TP-EDDA-COF also exhibited excellent substrate scope and recyclability. Comprehensive material characterization and theoretical calculations revealed that the enhanced planarity significantly facilitated charge separation and migration, thereby leading to improved photocatalytic efficiency. This study deepens the understanding of structure-activity relationships for COF photocatalysts, and provides a theoretical foundation for the rational design of high-performance photocatalysts for aerobic reactions.

共价有机骨架（COFs）的平面度是影响其光催化性能的重要结构参数。然而，其对光催化有机转化效率的影响尚未得到充分的研究。本文合成了三种不同平面度的β-酮胺COFs，分别为TP-EDDA-COF、TP-DATP-COF和TP-DMTP-COF，探讨了平面度对其光催化性能的影响。TP-EDDA-COF具有最佳的平面度，具有优越的可见光吸收范围和光生载流子分离和迁移效率。因此，它表现出优异的光催化性能，四氢喹啉（THQ）脱氢的转化率达到98%，苄胺（BA）氧化偶联的转化率达到99%。此外，TP-EDDA-COF还表现出良好的衬底范围和可回收性。综合材料表征和理论计算表明，平面度的增强显著促进了电荷的分离和迁移，从而提高了光催化效率。本研究加深了对COF光催化剂构效关系的认识，为合理设计用于好氧反应的高性能光催化剂提供了理论基础。

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引用次数: 0

Facile and green mechanochemical synthesis of highly stable vanadium-based heterogeneous catalyst for CO2-mediated oxidative dehydrogenation of propane 高稳定的钒基丙烷氧化脱氢多相催化剂的简易绿色机械化学合成

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-19 DOI: 10.1016/j.mcat.2025.115600

Yahya Gambo , Ariel H. Gursida , Akolade Idris Bakare , Sagir Adamu , Mohammed S. Ba-Shammakh , Mohammad. M. Hossain

Herein, we report the development of supported vanadium catalyst through a solvent-free mechanochemical route – a low-cost and green synthesis strategy – for CO₂-mediated oxidative dehydrogenation of propane. In the preliminary investigation, montmorillonite-supported VOx (MontV) and MgO-supported VOx (MgV) showed moderate propylene yields (19.6% and 18.2%, respectively) but with high CO selectivity at 625°C. Consequently, in the quest to harness possible synergy among the active components, other catalysts were rationally engineered via exploiting the manner of spatial integration of individual supports. Among the catalysts, Mont (MgV) derived via physical grinding of montmorillonite and MgV exhibited an excellent stable 31% yield to propylene without any noticeable deactivation over 12-hour time on stream. The structural changes of the catalytic surface and real-time evolution of the reaction intermediates were revealed with in-situ FTIR experiments. This work demonstrates a facile and highly scalable design template for engineering novel and efficient CO₂-ODH catalysts, adjudged as environmentally benign.

在此，我们报告了通过无溶剂机械化学途径-一种低成本和绿色合成策略-用于二氧化碳介导的丙烷氧化脱氢的负载型钒催化剂的开发。在初步研究中，蒙脱石负载的VOx （MontV）和氧化镁负载的VOx （MgV）在625℃时丙烯收率适中（分别为19.6%和18.2%），但CO选择性较高。因此，在寻求利用活性成分之间可能的协同作用的过程中，通过利用个体支撑的空间整合方式合理地设计了其他催化剂。在催化剂中，蒙脱土和MgV经物理研磨得到的Mont （MgV）的丙烯产率稳定在31%，在12小时内没有明显的失活现象。通过原位FTIR实验揭示了催化表面的结构变化和反应中间体的实时演化。这项工作展示了一种简单且高度可扩展的设计模板，用于工程设计新颖高效的CO2-ODH催化剂，被认为是环保的。

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引用次数: 0

Refining the surface O defect via Cu on WO3 hollow sphere for photocatalytic CO2 reduction 在WO3空心球上用Cu修饰表面O缺陷光催化CO2还原

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-19 DOI: 10.1016/j.mcat.2025.115596

Jilong Xiao , Yuxiang Li , Yuzhou Xia , Tuanyu Guo , Lu Chen , Shuying Zhu

Photocatalytic CO₂ reduction is a promising strategy for achieving carbon neutrality. Nevertheless, its efficiency is limited by the high energy barrier and severe charge recombination. Herein, Cu–WO₃ hollow sphere hybrids, in which Cu is anchored to the O defects of WO₃, were fabricated to enable efficient photocatalytic conversion of CO₂ to CO. The oxygen defects in WO₃ promote the preferential deposition of Cu, resulting in the simultaneous exposure of Cu–O defect active sites. In the engineered Cu–WO₃ structure, the confined hollow morphology improves CO₂ adsorption and facilitates the separation of photogenerated electrons and holes. The Cu–O defect centers effectively reduce the overpotential for CO₂ conversion. Consequently, the synthesized Cu–WO₃ catalyst demonstrates excellent and stable photocatalytic CO₂ reduction activity, achieving a CO production rate of 1518 μL g^–1 h^–1 in the absence of a sacrificial agent, which is 5.2 times greater than that of pristine WO₃. This study provides new insights into defect modulation for designing highly efficient photocatalytic materials.

光催化CO2还原是实现碳中和的一种很有前途的策略。然而，它的效率受到高能量势垒和严重的电荷复合的限制。本文制备了Cu - WO3空心球杂化物，其中Cu被锚定在WO3的O缺陷上，从而实现了CO2到CO的高效光催化转化。WO3中的氧缺陷促进了Cu的优先沉积，导致Cu - O缺陷活性位点同时暴露。在设计的Cu-WO3结构中，受限制的空心形貌提高了CO2的吸附能力，有利于光生电子和空穴的分离。Cu-O缺陷中心有效地降低了CO2转化的过电位。结果表明，制备的Cu-WO3催化剂具有良好稳定的光催化CO2还原活性，在不添加牺牲剂的情况下，Cu-WO3的CO产率为1518 μL g-1 h-1，是原始WO3的5.2倍。该研究为设计高效光催化材料提供了缺陷调制的新见解。

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引用次数: 0

Highly selective methoxycarbonylation of (R)-carvone with N-Xantphos-modified Pd-catalyst n -黄磷修饰pd催化剂对(R)-香芹酮的高选择性甲氧羰基化反应

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-15 DOI: 10.1016/j.mcat.2025.115595

Chen Chen , Pei-Ying Peng , Long-Gen Hu , Ying-Xi Hua , Ye Liu

An efficient and highly chemo/regioselective Pd-catalyzed methoxycarbonylation of biomass-based (R)-carvone has been established. Since there are several functional groups (like keto, cyclohexenyl) beside of isopropenyl in the scaffold of (R)-carvone, the numerous side-reactions derived from CC/CO double-bond isomerization will happen in parallel along with the required methoxycarbonylation, leading to the challenging control for the oriented generation of the targe carbonylated product. Herein, upon the careful ligand-selection and reaction condition optimization, the high conversion of (R)-carvone (95 %) with the excellent carbonylation-selectivity (95 %) were achieved, giving 90 % yield of the desired ester while the involved side-rection were successfully suppressed. It was noted that the process proved to be very chemo-/regio-selective by using the steric bulky and rigid biphosphine of N-Xantphos (L1) and MSA-acid-additive at the lower concentration.

建立了一种高效、高化学/区域选择性的pd催化生物质基香芹酮甲氧羰基化反应。由于(R)-香豆酮骨架中异丙烯旁边有几个官能团（如酮、环己烯基），因此CC/CO双键异构化产生的众多副反应将与所需的甲氧羰基化同时发生，导致定向生成目标羰基化产物的控制具有挑战性。通过对配体的精心选择和反应条件的优化，实现了(R)-香豆酮的高转化率（95%）和良好的羰基化选择性（95%），得到了90%的酯收率，同时成功抑制了所涉及的侧反应。在较低浓度下使用N-Xantphos （L1）和msa -酸添加剂的立体体积和刚性双膦，证明了该工艺具有很强的化学/区域选择性。

引用次数: 0

Maximizing framework titanium content in TS-1 zeolite through a novel boron extraction and titanium incorporation strategy 通过新型硼萃取和钛掺入策略最大化TS-1沸石骨架钛含量

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-15 DOI: 10.1016/j.mcat.2025.115597

Jinghui Lyu , Tao Liu , Shihao Wang, Jun Wei, Jinke Yao, Yiyong Zhao, Han Wu, Xianghao Zhang, Peikun Li, Zhizheng Wang, Qunfeng Zhang, Dahao Jiang, Qingtao Wang, Guofu Zhang, Chengrong Ding, Xiaonian Li

TS-1 zeolite is a catalyst known for its high selective oxidation performance and broad industrial applications. The titanium atom in the TS-1 often acts as the active center in catalytic reactions, especially in oxidation reactions, so increasing the titanium content in TS-1 is of great significance in chemical reactions and catalytic applications. This paper explores a Novel Boron Extraction and Titanium Incorporation Strategy to enhance the titanium content within the TS-1 framework. During the dry gel preparation process, boron species were introduced in situ into the framework of the TS-1 to form a framework boron-titanium-silicon TS-1-B with tetra-coordinated or tri-coordinated positions. TS-1-B is then treated with acid to remove the framework boron, while an appropriate amount of titanium precursor is introduced to fill the vacancy left by the removal of the framework boron. The results of XRD, FT-IR, UV–Vis, BET, NH₃-TPD, XRF, and XPS showed that the titanium content of the tetracoordinate framework in the TS-1 was improved. The catalytic performances of TS-1-B, TS-1-BS, and TS-1-BST were comparatively evaluated through two representative reactions: propylene epoxidation and the direct synthesis of hydrogen peroxide from H₂ and O₂.

TS-1沸石是一种催化剂，以其高选择性氧化性能和广泛的工业应用而闻名。TS-1中的钛原子在催化反应特别是氧化反应中经常作为活性中心，因此提高TS-1中钛的含量在化学反应和催化应用中具有重要意义。本文探讨了一种新的提硼钛掺入策略，以提高TS-1框架下的钛含量。在干凝胶制备过程中，将硼种原位引入TS-1骨架中，形成四配位或三配位的硼钛硅骨架TS-1- b。然后对TS-1-B进行酸处理去除骨架硼，同时加入适量钛前驱体填补骨架硼去除后留下的空位。XRD、FT-IR、UV-Vis、BET、NH3-TPD、XRF、XPS等测试结果表明，TS-1中四坐标骨架的钛含量有所提高。通过丙烯环氧化反应和由H₂和O₂直接合成过氧化氢两个代表性反应，比较评价了TS-1-B、TS-1-BS和TS-1-BST的催化性能。

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引用次数: 0

Hydrogen spillover-induced low-temperature activation of NiCu/Al₂O₃ catalyst for efficient polyalphaolefin hydrogenation 氢外溢诱导NiCu/Al₂O₃催化剂低温活化高效加氢聚α -烯烃

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-14 DOI: 10.1016/j.mcat.2025.115598

Jie Wang , Yilong Chen , Chengxi Zhang , Xuan Meng , Naiwang Liu , Li Shi

To our knowledge, this is the first time the Ni_xCu_y/Al₂O₃ catalyst has been prepared by the deposition-precipitation method and applied to the hydrogenation synthesis of polyalphaolefins (PAO). The effects of the Ni/Cu molar ratio, catalyst preparation conditions, and reduction temperature on the hydrogenation performance of these catalysts were systematically investigated. The 200 °C low-temperature reduction strategy effectively inhibited the sintering of active sites, thereby significantly improving metal dispersion and reducibility. The characterization results show that the introduction of Cu promotes the dispersion of Ni and the activation ability of H₂. Combined with the synergistic effect of the mesoporous Al₂O₃ carrier, the structure of the catalyst is optimized. Among these catalysts, Ni₃Cu₁/Al₂O₃ exhibits the optimal hydrogenation activity and stability under low-temperature reduction conditions. This superiority is attributed to the hydrogen spillover effect of Cu, which promotes the migration of active hydrogen to Ni sites and thus reduces the reaction energy barrier. This catalyst still maintains high activity and stability under high space velocity conditions, demonstrating a promising industrial application prospect.

据我们所知，这是第一次用沉积-沉淀法制备NixCuy/Al2O3催化剂，并将其应用于聚α烯烃（PAO）的加氢合成。系统考察了Ni/Cu摩尔比、催化剂制备条件和还原温度对催化剂加氢性能的影响。200℃低温还原策略有效抑制了活性位点的烧结，从而显著提高了金属的分散性和还原性。表征结果表明，Cu的引入促进了Ni的分散和H2的活化能力。结合介孔Al2O3载体的协同作用，对催化剂的结构进行优化。其中，Ni3Cu1/Al2O3在低温还原条件下表现出最佳的加氢活性和稳定性。这种优势归因于Cu的氢溢出效应，它促进了活性氢向Ni位点的迁移，从而降低了反应能垒。该催化剂在高空速条件下仍保持较高的活性和稳定性，具有良好的工业应用前景。

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引用次数: 0

Exploring Ni nanoparticles: Progress and future perspectives in organic transformations 探索纳米镍：有机转化的进展和未来展望

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-14 DOI: 10.1016/j.mcat.2025.115567

Rashika , Tannavi Badhan , Deepika Thakur , Akhilesh K. Verma , Sushmita

The diverse applications of nanoparticles make the construction of the various scaffolds which fascinates the interest of synthetic chemists for exploitation. Among the metals, nickel is cheaper and environmentally benign which has gained considerable attention with the emergence of newer methods and is advantageous in terms of their availability, ease of handling, and excellent recyclability. This review comprehensively summarizes the significant advances and scopes of nickel nanoparticles being employed as sustainable and non-precious catalytic protocol with high-performance catalysts on developments of organic synthetic chemistry that offer an opportunity to overcome obstacles in the pharmaceuticals and industries. This review comprehensively highlights the (2010–2024) article that focuses on the methods of preparation of Ni-NPs and emphasizes on different organic synthetic methodologies. In this review, we provide an overview of the recent progress, challenges, opportunities, and future outcomes in the area of nanoparticle chemistry using cheap nickel nanoparticles available as a Ni(0) source.

纳米颗粒的多种应用使得各种支架的构建引起了合成化学家的兴趣。在金属中，镍的价格较低，对环境无害，随着新方法的出现而引起了相当大的关注，并且在可获得性、易于处理和极好的可回收性方面具有优势。本文综述了纳米镍在有机合成化学发展中作为可持续的、非贵重的催化剂和高性能催化剂的重大进展和范围，为克服制药和工业中的障碍提供了机会。本文综合介绍了（2010-2024）Ni-NPs的制备方法，重点介绍了不同的有机合成方法。在这篇综述中，我们概述了利用廉价的镍纳米颗粒作为Ni(0)源的纳米颗粒化学领域的最新进展、挑战、机遇和未来成果。

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引用次数: 0

Ce doping enhances MOF-derived rod shape CoOx/MnOx catalysts for photothermocatalytic degradation of 1,2-Propanediol and NO without ammonia Ce掺杂增强了mof衍生棒状CoOx/MnOx催化剂光热催化降解1,2-丙二醇和NO的性能

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2025-11-14 DOI: 10.1016/j.mcat.2025.115604

Yinming Fan , Siqi Jiang , Yanzhen Li , Yanping Zhang , Yinian Zhu , Shengpeng Mo , Lei Liao , Yanan Zhang , Xiaobin Zhou , Zongqiang Zhu

This study designed a series of MOF-derived rod shape CoO_x/MnO_x and CeO₂/CoO_x/MnO_x catalysts by optimizing the Co/Mn molar ratio and Ce doping level for the synergistic photothermal catalytic degradation of NO and 1,2-propanediol. When n_Co:n_Mn = 5:1, the catalyst achieved the highest conversion rates for NO and 1,2-propanediol at 240 °C, reaching 78.68 % and 68 %, respectively. Further doping with Ce, specifically at n_Co−_Mn:n_Ce = 1:0.2, yielded the highest conversion rates of 86 % for NO and 77 % for 1,2-propanediol at 240 °C. Through a series of characterizations, the core effects of Ce doping were identified as: enhancing oxygen vacancy concentration, improving redox capability, inducing lattice distortion and active site exposure, optimizing electronic structure. XAFS analysis reveals that Ce doping induces lattice distortion, reduces Co-Co coordination number, and increases Mn⁴⁺ proportion, enhancing oxygen vacancy concentration and redox capability. Finally, the reaction pathway of photothermocatalysis was elucidated based on in-situ DRIFTS. This work provides a new strategy for Ce-modulated bimetallic oxide catalysts for the synergistic removal of volatile organic pollutants and nitrogen oxides.

本研究通过优化Co/Mn摩尔比和Ce掺杂水平，设计了一系列mof衍生的棒状CoOx/MnOx和CeO2/CoOx/MnOx催化剂，用于协同光热催化降解NO和1,2-丙二醇。当nCo:nMn = 5:1时，催化剂在240℃时对NO和1,2-丙二醇的转化率最高，分别达到78.68%和68%。进一步掺杂Ce，特别是在nCo−Mn:nCe = 1:0.2时，在240℃下，NO的转化率为86%，1,2-丙二醇的转化率为77%。通过一系列表征，确定了Ce掺杂的核心效应为：提高氧空位浓度、提高氧化还原能力、诱导晶格畸变和活性位点暴露、优化电子结构。XAFS分析表明，Ce掺杂引起晶格畸变，降低Co-Co配位数，增加Mn4+比例，提高氧空位浓度和氧化还原能力。最后，基于原位漂移技术，阐明了光热催化的反应途径。本研究为铈调制双金属氧化物催化剂协同去除挥发性有机污染物和氮氧化物提供了一种新的策略。

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引用次数: 0