Molecular Catalysis最新文献_第3页

Chiral thiol-anchored L-proline self-assembled monolayers on Pd-decorated Fe3O4 nanocomposites for one-pot oxidation–aldol reactions and sequential reduction 手性硫醇锚定l-脯氨酸自组装单层在pd修饰的Fe3O4纳米复合材料中一锅氧化-醛反应和顺序还原

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-28 DOI: 10.1016/j.mcat.2026.115738

Sanjiv O. Tomer , Jagrut Barot , Sudhirkumar S. Katariya , Rudresh J. Shah , Sanjay N. Bariya , Saurabh S. Soni , Hemant P. Soni

Self-assembled chiral interfaces on heterogeneous catalysts provide a powerful strategy for integrating redox and enantioselective transformations within a single catalytic platform. Herein, we report the rational design of a multifunctional SAM-functionalized Pd-decorated Fe₃O₄ nanocatalyst (Fe₃O₄@Pd@SAM), in which superparamagnetic Fe₃O₄ nanospheres enable facile recovery, surface-accessible Pd domains mediate redox processes, and a densely packed thiol-anchored l-proline self-assembled monolayer imparts chiral induction. Comprehensive structural and surface characterization by PXRD, HRTEM, AFM, FTIR, SERS, and XPS depth profiling demonstrates the formation of a Pd-enriched interfacial architecture with a highly ordered chiral SAM confined to the outermost surface. Electrochemical studies reveal efficient interfacial charge transfer and enhanced redox accessibility relative to Pd@SAM and free ligand systems, highlighting the cooperative role of the Pd/SAM interface. The nanocatalyst efficiently promotes a one-pot aerobic oxidation–asymmetric aldol reaction of benzyl alcohols and ketones under mild, green conditions, delivering β‑hydroxy ketones with excellent yields and enantioselectivities (up to 100% ee in selected cases). Importantly, the robustness of the chiral interface enables extension of the process to a sequential reduction step performed in the same reaction vessel, affording optically active α-alkylated benzyl alcohols. The catalyst exhibits high recyclability, maintains stereochemical fidelity over multiple cycles, and demonstrates applicability at the pilot scale. This study highlights SAM-functionalized Pd-decorated Fe₃O₄ nanocomposites as versatile platforms for integrating heterogeneous redox catalysis with asymmetric organocatalysis in sustainable catalytic systems.

多相催化剂上的自组装手性界面为在单一催化平台内整合氧化还原和对映选择性转化提供了强有力的策略。在此，我们报告了一种多功能sam功能化Pd修饰的Fe3O4纳米催化剂（Fe3O4@Pd@SAM）的合理设计，其中超顺磁性Fe3O4纳米球易于回收，表面可访问的Pd结构域介导氧化还原过程，密集排列的硫醇锚定的l-脯氨酸自组装单层赋予手性诱导。通过PXRD， HRTEM， AFM， FTIR， SERS和XPS深度谱分析，综合结构和表面表征表明形成了富含pd的界面结构，其最外层表面具有高度有序的手性SAM。电化学研究表明，相对于Pd@SAM和自由配体体系，Pd/SAM具有高效的界面电荷转移和增强的氧化还原可及性，突出了Pd/SAM界面的协同作用。该纳米催化剂在温和的绿色条件下，有效地促进了苯甲醇和酮类的一锅有氧氧化-不对称醛醇反应，产生了具有优异收率和对映选择性的β -羟基酮（在某些情况下高达100% ee）。重要的是，手性界面的鲁棒性使得该过程可以在同一反应容器中连续还原步骤，从而获得光学活性α-烷基化苄基醇。该催化剂具有高可回收性，在多次循环中保持立体化学保真度，并在中试规模上证明了适用性。这项研究强调了sam功能化pd修饰的Fe3O4纳米复合材料作为多功能平台，可以在可持续的催化系统中整合多相氧化还原催化和不对称有机催化。

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引用次数: 0

A high-performance cryptomelane-type MnO2 synthesized by one-step hydrothermally method for low-temperature NO conversion with NH3 一步水热法合成高性能隐黑烷型二氧化锰，用于NH3低温NO转化

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-28 DOI: 10.1016/j.mcat.2026.115743

Guanghui Li , Xiduan Yang , Sizhe Luo , Changye Mang , Jun Luo , Mingjun Rao

The development of high-performance catalysts for low-temperature selective catalytic reduction of NO_x with NH₃ (NH₃-SCR) is crucial for advancing industrial flue gas denitrification. In this study, cryptomelane-type α-MnO₂ catalysts were synthesized via a facile one-step hydrothermal method. It was demonstrated that precise control of the hydrothermal temperature and duration effectively tailors the catalyst’s physicochemical properties, including Mn³⁺/Mn⁴⁺ ratio, oxygen vacancy concentration, and Brønsted acid site density. The optimally synthesized catalyst (Cry-240-1h) exhibits exceptional low-temperature SCR activity, achieving 96 % NO conversion at 200°C under simulated flue gas conditions (500 ppm NO, 1000 ppm NH₃, 5 % O₂, 5 % H₂O, GHSV = 36,000 h^-1). This performance surpasses that of analogous catalysts prepared by conventional multi-step hydrothermal-roasting methods. The superior activity is attributed to the synergistic enhancement of redox properties (from abundant Mn³⁺ and oxygen vacancies) and surface acidity (dominant Brønsted acid sites), which facilitate the adsorption and activation of both NH₃ and NO. This work provides a rational and efficient strategy for designing high-performance Mn-based low-temperature SCR catalysts through simple synthesis parameter optimization.

开发高性能的NH3低温选择性催化还原NOx催化剂（NH3- scr）是推进工业烟气脱硝的关键。本研究采用简单的一步水热法合成了隐黑烷型α-MnO2催化剂。结果表明，精确控制水热温度和持续时间可以有效地调整催化剂的物理化学性质，包括Mn3+/Mn4+比、氧空位浓度和Brønsted酸位密度。最佳合成的催化剂（crry -240-1h）表现出优异的低温SCR活性，在模拟烟气条件下（500 ppm NO, 1000 ppm NH3, 5% O2, 5% H2O, GHSV = 36,000 h-1），在200°C下实现96%的NO转化率。该性能优于传统多步水热焙烧法制备的类似催化剂。这种优异的活性是由于氧化还原性能（来自丰富的Mn3+和氧空位）和表面酸度（主要的Brønsted酸位点）的协同增强，从而促进了NH3和NO的吸附和活化。本研究为通过简单的合成参数优化设计高性能锰基低温SCR催化剂提供了合理有效的策略。

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引用次数: 0

Highly selective hydrodeoxygenation of lignin and its derivatives to cyclohexanols over N-doped nickel catalyst without external hydrogen 木质素及其衍生物在n掺杂镍催化剂上无外氢高选择性加氢脱氧制环己醇

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-27 DOI: 10.1016/j.mcat.2026.115742

Meiyan Shi , Qibin Zeng , Ting Pan , Yuancai Lv , Yifan Liu , Minghua Liu

Transforming lignin into cyclohexanol through catalytic processes is crucial for the development of next-generation biofuels. Nevertheless, realizing highly selective hydrogenation-deoxygenation depolymerization under mild reaction conditions continues to pose a considerable challenge. Herein, a nitrogen-doped carbon-supported nickel catalyst (Ni@NC) was developed and successfully applied to the depolymerization of lignin. Characterization results revealed that the catalyst possesses a rich porous structure and moderate metal–support interactions, contributing to its remarkable catalytic performance. Under mild conditions (200 °C, without external hydrogen and pressure), Ni@NC-600 achieved 100% conversion of the model compound PPE with a 99.5% yield of cyclohexanol. At 250 °C, it also enabled 98.7% depolymerization of lignin within 5 h, yielding 21.36 wt% of naphthenes and their derivatives. Theoretical calculations further confirmed that nitrogen doping facilitates electron transfer between the support and nickel nanoparticles. The reconfigured electronic environment significantly enhanced the catalyst's adsorption capacity for phenolic compounds, thereby improving its hydrogenation performance. This work not only provides a viable pathway for the high-value conversion of lignin but also offers an innovative strategy for electronic structure design in catalyst development.

通过催化过程将木质素转化为环己醇对于开发下一代生物燃料至关重要。然而，在温和反应条件下实现高选择性加氢-脱氧解聚仍然是一个相当大的挑战。本文开发了一种氮掺杂碳负载镍催化剂（Ni@NC），并成功应用于木质素的解聚。表征结果表明，该催化剂具有丰富的多孔结构和适度的金属-载体相互作用，具有优异的催化性能。在温和的条件下（200°C，无外部氢气和压力），Ni@NC-600实现了模型化合物PPE 100%的转化率，环己醇收率为99.5%。在250℃下，它也使木质素在5 h内解聚98.7%，产生21.36%的环烷及其衍生物。理论计算进一步证实，氮掺杂促进了载体和纳米镍之间的电子转移。重新配置的电子环境显著增强了催化剂对酚类化合物的吸附能力，从而提高了催化剂的加氢性能。这项工作不仅为木质素的高价值转化提供了一条可行的途径，而且为催化剂开发中的电子结构设计提供了一种创新策略。

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引用次数: 0

Constructing S-Cu₂O/Cu interfaces via electrochemical deposition for selective reduction of CO₂ to formate 通过电化学沉积构建S-Cu₂O/Cu界面，选择性还原CO₂生成甲酸

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-27 DOI: 10.1016/j.mcat.2026.115715

Kai Hu, Lin Li, Congya Wang, Jing Zhang, Hexiang Zhong, Liwei Pan

The electrochemical reduction of CO₂ (ERCO₂) to value-added chemicals offers a promising approach for carbon mitigation and renewable energy storage. However, achieving both high selectivity and high current density toward formic acid remains challenging. Here, we report a sulfur-modified Cu catalyst (Cu-S_(P/R)) synthesized via a two-step electrochemical strategy combining pulsed electrodeposition (PED) with constant-potential reconfiguration (CPR). During PED, sulfur incorporation into the Cu₂O/Cu surface, followed by CPR-driven in situ reconstruction, generates highly active S-modified Cu₂O/Cu interfacial sites and simultaneously modulates the surface structures of the catalyst. Thus, the optimized Cu-S_(P/R) catalyst delivers a maximum Faradaic efficiency of 85.7 %, with a partial current density of 20.86 mA/cm². This work offers a promising strategy for developing highly efficient ERCO₂ electrocatalysts.

电化学还原CO₂（ERCO₂）为增值化学品提供了一种有前途的碳减排和可再生能源储存方法。然而，实现对甲酸的高选择性和高电流密度仍然具有挑战性。本文报道了一种硫修饰铜催化剂（Cu- s (P/R)），通过脉冲电沉积（PED）和恒电位重构（CPR）两步电化学策略合成。在PED过程中，硫进入Cu₂O/Cu表面，随后进行cpr驱动的原位重构，产生高活性的s修饰Cu₂O/Cu界面位点，同时调节催化剂的表面结构。因此，优化后的Cu-S（P/R）催化剂的最大法拉第效率为85.7%，分电流密度为20.86 mA/cm²。这项工作为开发高效ERCO₂电催化剂提供了一个有前途的策略。

引用次数: 0

Spatially decoupled Cu/SiO2|CoMn catalyst enhances syngas conversion to higher oxygenates 空间解耦的Cu/SiO2催化剂提高合成气转化为高氧化物

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-24 DOI: 10.1016/j.mcat.2026.115745

Su Li , Bin Chai , Lei Guo , Yingjun Wang , Kegong Fang

Direct conversion of syngas to higher oxygenates remains a considerable challenge due to the complicated reaction network. Here, we develop a spatially decoupled Cu/SiO₂|CoMn (granule-stacked) multifunctional catalyst with superior catalytic performance, exhibiting 50.5% oxygenates selectivity (C₂₊OH/ROH=95.2%) with low C₁ byproducts formation (10.1% CO₂ and 4.5% CH₄) at 13.2% CO conversion. The spatially decoupled configuration synergistically integrates the distinct active sites between the Cu/SiO₂ and CoMn components by precisely optimizing the proximity and mass ratios, thereby steering the reaction network with high efficiency. Based on spectroscopic results, the synergistic mechanism reveals that the intrinsic role of Cu⁰ sites is responsible for generating CH_xO* species, which then migrate to the Co⁰-Co₂C interfaces, couple with CH_x* species, and thereby boost the oxygenates formation.

由于反应网络复杂，合成气直接转化为高氧化合物仍然是一个相当大的挑战。在此，我们开发了一种空间解耦的Cu/SiO2|CoMn（颗粒堆）多功能催化剂，具有优异的催化性能，具有50.5%的氧选择性（C2+OH/ROH=95.2%）和低C1副产物（10.1% CO2和4.5% CH4）， 13.2%的CO转化率。空间解耦结构通过精确优化接近度和质量比，协同整合Cu/SiO2和common组分之间不同的活性位点，从而高效地控制反应网络。基于光谱结果，协同机制揭示了Cu0位点的内在作用是产生CHxO*物质，然后迁移到co - co2c界面，与CHx*物质偶联，从而促进氧合物的形成。

引用次数: 0

Exploring the influence of acid etching on the active sites of Pd/Al2O3 catalyst for toluene combustion: Regulation of defects 探索酸蚀对Pd/Al2O3甲苯燃烧催化剂活性位点的影响：缺陷的调控

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-24 DOI: 10.1016/j.mcat.2026.115744

Teng Liu , Junwei Xu , Yi Pei , Junhua Cao , Xianglan Xu , Xiuzhong Fang , Jiating Shen , Xiang Wang

Pd/Al₂O₃-A_x catalysts were synthesized by etching the γ-Al₂O₃ support with nitric acid and subsequently loading Pd onto it. This series of catalysts was employed for toluene combustion. As the degree of acid etching increased, the performance of the catalysts improved. NH₃-TPD and in situ DRIFTS of NH₃ adsorption results indicated that acid etching increased the concentration of Lewis acid sites, thereby enhancing the adsorption and activation of toluene molecules. Meanwhile, FTIR, H₂-TPR, and EPR results suggested that acid etching introduced vacancies on the catalyst surface, while O₂-TPD and ¹⁸O₂-TPSR-MS results confirmed the enhanced oxygen activation ability of the catalyst. The synergistic effects of these factors improved the catalytic toluene combustion performance.

用硝酸蚀刻γ-Al2O3载体，然后在载体上加载Pd，合成了Pd/Al2O3-Ax催化剂。该系列催化剂用于甲苯燃烧。随着酸蚀程度的增加，催化剂的性能也随之提高。NH3- tpd和NH3原位漂移吸附结果表明，酸蚀增加了Lewis酸位点的浓度，从而增强了甲苯分子的吸附和活化。同时，FTIR、H2-TPR和EPR结果表明酸蚀在催化剂表面引入了空位，O2-TPD和18O2-TPSR-MS结果证实了催化剂氧活化能力的增强。这些因素的协同作用提高了甲苯的催化燃烧性能。

引用次数: 0

Precise elucidation of the structure-activity relationship between anatase TiO2 facets and surface active sites of V2O5-WO3/TiO2 catalysts for the NH3-selective catalytic reduction of NO nh3选择性催化还原NO的V2O5-WO3/TiO2催化剂表面活性位点与锐钛矿TiO2切面构效关系的精确解析

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-24 DOI: 10.1016/j.mcat.2026.115746

Jianyou Liang , Ling Yang , Bolian Xu , Haiqin Wan , Yubing Liu , Lei Yu , Yining Fan

A series of V₂O₅-WO₃/TiO₂ catalysts were synthesized using anatase TiO₂ supports predominantly exposing the {001}, {101} and {111} facets. Their performance in the selective catalytic reduction (SCR) of NO_x was evaluated, revealing that WO₃ acts as an effective promoter, enhancing the catalytic activity across all catalysts. However, the promotional mechanism was found to be strongly dependent on the exposed facet of the TiO₂ supports. The SCR activity followed the order: V₂O₅-WO₃/TiO₂-NS{001} > V₂O₅-WO₃/TiO₂-NP{101} > V₂O₅-WO₃/TiO₂-NL{111}. Characterization of surface acidity and redox properties indicated that the introduction of WO₃ increased the amount of weak B acid sites, thereby contributing to the enhanced SCR performance. Combining experimental and theoretical analyses revealed that the exposed facet of the TiO₂ support modulates the acidic strength of surface W⁶⁺ ions. Specifically, W⁶⁺ ions dispersed within the octahedral vacancies of the TiO₂-NS{001} surface exhibited the lowest Bader positive charge, corresponding to the weakest surface acidity. This accounts for the superior SCR performance of the V₂O₅-WO₃/TiO₂-NS{001} catalyst. This study elucidates the intrinsic relationship between the preferentially exposed facets of anatase TiO₂ supports and the surface acidity of W⁶⁺ ions in V₂O₅-WO₃/TiO₂ catalysts, providing a critical theoretical foundation and practical guidance for the rational design and optimization of high-efficiency SCR catalysts for NO_x abatement.

以锐钛矿型TiO2为载体，主要暴露{001}、{101}和{111}面，合成了一系列V2O5-WO3/TiO2催化剂。在选择性催化还原（SCR） NOx过程中，WO3作为一种有效的促进剂，提高了所有催化剂的催化活性。然而，促进机制被发现强烈依赖于TiO2载体的暴露面。SCR活性依次为：V2O5-WO3/TiO2-NS{001} >； V2O5-WO3/TiO2-NP{101} > V2O5-WO3/TiO2-NL{111}。表面酸度和氧化还原性能的表征表明，WO3的引入增加了弱B酸位点的数量，从而有助于提高SCR性能。结合实验和理论分析发现，TiO2载体的暴露面调节了表面W6+离子的酸性强度。具体来说，分散在TiO2-NS{001}表面八面体空位内的W6+离子表现出最低的Bader正电荷，对应于最弱的表面酸度。这是V2O5-WO3/TiO2-NS{001}催化剂具有优异SCR性能的原因。本研究阐明了锐钛矿型TiO2载体优先暴露面与V2O5-WO3/TiO2催化剂中W6+离子表面酸度之间的内在关系，为合理设计和优化高效SCR脱硝催化剂提供了重要的理论基础和实践指导。

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引用次数: 0

Diamondoid ketones as structural probes for active sites of fungal enzymes 金刚石酮作为真菌酶活性位点的结构探针

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-22 DOI: 10.1016/j.mcat.2026.115741

Valeriia V. Nikitenkova , Wendell Albuquerque , Martin Gand , Stefan Janssen , Binglin Li , Holger Zorn , Tatyana S. Zhuk

To reveal the enzymes active sites, the oxidative activities of twelve wood-degrading fungi was tested using rigid adamantanone and diamantanone models that contain clearly defined hydrophobic and hydrophilic regions. Fungal cultures have been observed to exhibit three distinct catalytic behaviors, namely, exclusively carbonyl-reductive activity, exclusively C–H oxidative activity, or a combination of both. The two most promising fungi, Cerrena zonata and Wolfiporia cocos were selected for aerobic on-water preparative oxidations during which series of diols and hydroxyketones were produced and characterized. To identify the enzymes responsible for these transformations, experiments using fungal mycelia were performed. Mycelium of C. zonata exhibited oxidative activity only when the culture was supplemented with the model compound 24 h prior to mycelium separation; in the absence of supplementation, no activity was detected. In contrast, transformations using mycelium from both supplemented and non-supplemented cultures of W. cocos did not yield any products. To identify genes potentially involved in the biotransformation, a comparative transcriptomic analysis of supplemented and non-supplemented C. zonata cultures was performed. Based on BLAST analysis and molecular docking studies, two candidate enzymes potentially responsible for the oxidation process were identified. These findings lay the groundwork for unraveling the enzymatic mechanisms that drive hydrocarbon oxidation in wood-rot fungi and pave the way for future characterization and development of biocatalysts.

为了揭示酶的活性位点，采用刚性金刚烷酮和金刚烷酮模型测试了12种木材降解真菌的氧化活性，这些模型包含明确定义的疏水性和亲水性区域。已经观察到真菌培养物表现出三种不同的催化行为，即完全羰基还原活性，完全C-H氧化活性，或两者的结合。选择了两种最有前途的真菌，Cerrena zonata和Wolfiporia cocos进行了好氧水制备氧化，在此过程中产生了一系列二醇和羟酮并进行了表征。为了确定负责这些转化的酶，使用真菌菌丝进行了实验。只有在菌丝分离前24 h添加模型化合物时，棘球绦虫菌丝才表现出氧化活性；在没有补充的情况下，没有检测到活性。相比之下，使用补充和未补充的椰子树菌丝体进行转化都没有产生任何产物。为了鉴定可能参与生物转化的基因，对补充和未补充的褐藻培养物进行了比较转录组学分析。基于BLAST分析和分子对接研究，确定了两种可能负责氧化过程的候选酶。这些发现为揭示木腐真菌中驱动碳氢化合物氧化的酶机制奠定了基础，并为未来生物催化剂的表征和开发铺平了道路。

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引用次数: 0

Biotemplated construction of CoCu/Bio-CeO2 for efficiently boosting the tandem hydrogenation of nitroaromatics CoCu/Bio-CeO2生物模板化构建高效促进硝基芳烃的串联加氢反应

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-21 DOI: 10.1016/j.mcat.2026.115734

Zhiyong Fu , Xusheng Yang , Sirong Zhao , Shun Hu , Changsong Chen , Bin Xu , Zhen Xiang , Weidong Jiang

Tea pollen-template fabricated Bio-CeO₂ served as a support for developing the supported CoCu-based bimetallic catalysts (CoCu/Bio-CeO₂). The catalytic performance of the as-prepared CoCu/Bio-CeO₂ catalysts was evaluated in the tandem hydrogenation of nitroaromatic compounds. The templated Bio-CeO₂ support not only successfully replicates the natural porous structure of tea pollen, but also induces the catalyst reconstruction and compositional differentiation. In contrast to non-templated or sole metallic analogues, Bio-CeO₂-supported CoCu-based nanocatalysts endow more promising catalytic performance. The one selected Co₁Cu₄/Bio-CeO₂ exhibited excellent reactivity, achieving a hydrogen production rate (HGR) of 422.2 mL·min⁻¹·gcat⁻¹ and a nearly 99% yield of m-chloraniline (m-CAN) in the in-situ hydrogenation of m-chloronitrobenzene (m-CNB) under mild conditions. High activity was remained accompanying with over 87% yield of m-CAN after six runs. Co₁Cu₄/Bio-CeO₂ displayed superior activity and good substrate adaptability in the tandem hydrogenation of aromatic nitro compounds bearing various functional groups. The high stability and desired catalytic performance of Co₁Cu₄/Bio-CeO₂ shall be attributed to intermetallic synergistic effect as well as strong interaction between active metal and the Bio-CeO₂ support.

茶花粉模板制备的Bio-CeO 2作为载体，用于开发负载型CoCu基双金属催化剂（CoCu/Bio-CeO 2）。对制备的CoCu/Bio-CeO 2催化剂在硝基芳香族化合物串联加氢反应中的催化性能进行了评价。模板化的bio - ceo2载体不仅成功复制了茶花粉的天然多孔结构，而且诱导了催化剂的重构和成分分化。与非模板或单一金属类似物相比，bio - ceo2负载的cocu基纳米催化剂具有更有前景的催化性能。所选择的Co₁Cu₄/Bio-CeO₂具有良好的反应活性，在温和的条件下，对间氯硝基苯（m-CNB）进行原位加氢，产氢率（HGR）为422.2 mL·min⁻¹·gcat⁻¹，间氯苯胺（m-CAN）的产率接近99%。6次处理后，m-CAN酶活性保持在87%以上。Co₁Cu₄/Bio-CeO₂对含各种官能团的芳香硝基化合物的串联加氢表现出优异的活性和良好的底物适应性。Co₁Cu₄/Bio-CeO₂的高稳定性和理想的催化性能应归功于金属间协同效应以及活性金属与Bio-CeO₂载体之间的强相互作用。

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引用次数: 0

Breaking the energy bottleneck in amine regeneration: Fe-HZSM-5 catalysts with tunable acid sites for high-performance CO₂ desorption 打破胺再生的能量瓶颈：具有可调酸位的Fe-HZSM-5催化剂用于高性能CO₂脱附

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis

Pub Date : 2026-01-21 DOI: 10.1016/j.mcat.2026.115736

Bin Wang , Weigao Han , Fang Dong , Hua Feng , Zhicheng Tang

The substantial energy consumption required for rich amine solution regeneration significantly constrains its industrial application. The development of solid acid catalysts has become a key approach to addressing this issue. Herein, different types and loadings of metal-modified HZSM-5 catalysts by ultrasound-assisted impregnation were prepared to optimize the catalytic performance for CO₂ desorption from monoethanolamine (MEA) solution. The characterization showed that different types of metal ions had a significant influence on the morphology of catalysts and the metal modification successfully regulated the distribution of acid sites. The result showed that Fe-HZSM-1/6 achieved the best performance. The maximum desorption rate could reach 29.17 mmol·min^-1·L^-1 (161 % higher than the blank), the total amount of desorbed CO₂ increased by 38%, and the relative heat duty decreased by 27%. The Py-IR and NH₃-TPD analysis indicated that the Fe-HZSM-1/6 catalyst provides abundant Brønsted acid centers and Lewis acid centers, which can synergistically promote proton transfer and the decomposition of carbamates. This catalyst still maintains 84 % of its activity after 5 cycles. This work highlights the key role of acidic site regulation in amine regeneration and provides a rational design strategy for low-energy consumption catalysts.

富胺溶液再生所需的大量能源消耗极大地制约了其工业应用。开发固体酸催化剂已成为解决这一问题的关键途径。本文采用超声辅助浸渍法制备了不同类型和负载的金属改性HZSM-5催化剂，以优化其在单乙醇胺（MEA）溶液中解吸CO2的催化性能。表征表明，不同类型的金属离子对催化剂的形貌有显著的影响，金属改性成功地调节了酸位的分布。结果表明，Fe-HZSM-1/6具有最佳性能。最大解吸速率可达29.17 mmol·min-1·L-1（比空白提高161%），解吸CO2总量提高38%，相对热负荷降低27%。Py-IR和NH3-TPD分析表明，Fe-HZSM-1/6催化剂提供了丰富的br - nsted酸中心和Lewis酸中心，可以协同促进质子转移和氨基甲酸酯的分解。该催化剂经过5次循环后仍保持84%的活性。这项工作突出了酸性位点调控在胺再生中的关键作用，并为低能耗催化剂的合理设计提供了策略。

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引用次数: 0