Applied Catalysis A: General最新文献_第5页

Study on the effects of Nd-doping on the performance of Cu-based CO2 hydrogenation catalysts with different oxide supports nd掺杂对不同氧化物载体cu基CO2加氢催化剂性能影响的研究

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-22 DOI: 10.1016/j.apcata.2025.120757

Shuai Hu , Xiaoxuan Zhu , Yan Zhu , Chenliang Zhou , Gewen Yu , Yanming Wang , Cong Wang , Zhenfeng Wang , Jian Ding , Yuqing Wang , Xiaohui Guo

To enhance the activity and selectivity of Cu-based catalysts in the CO₂ hydrogenation reaction, this study systematically investigated the regulation effect of Nd-doping on the structure and surface properties of different oxide support (MgO, Al₂O₃, ZrO₂, and CeO₂), and further explored its influence on the state of Cu species as well as the catalytic performance in CO₂ hydrogenation to methanol. The results show that the introduction of Nd^3 + can effectively induce lattice distortion of the support which promotes the generation of oxygen vacancies and the formation of surface basic sites, thereby enhancing the interfacial electronic interaction between Cu and support and improving the stability of Cu⁺ active centers. Among them, the Cu catalyst supported on Nd-doped ZrO₂ exhibited the best catalytic performance such as the high CO₂ conversion and selectivity to methanol. Various characterization (XRD, SEM, in-situ XPS, H₂-TPR, CO₂-TPD, and H₂-TPD) results confirmed the key role of Nd-doping in regulating the oxygen defects, electronic structure, and Cu species distribution over support. This study reveals the structural regulation mechanism of Nd in constructing efficient Cu-based catalysts for CO₂ hydrogenation from the perspective of support engineering, providing theoretical basis and practical guidance for the design of new high-performance catalytic materials.

为了提高Cu基催化剂在CO2加氢反应中的活性和选择性，本研究系统研究了nd掺杂对不同氧化物载体（MgO、Al2O3、ZrO2和CeO2）结构和表面性质的调控作用，并进一步探讨了其对Cu态的影响以及对CO2加氢制甲醇催化性能的影响。结果表明，Nd3 +的引入能有效诱导载体的晶格畸变，促进氧空位的生成和表面基位的形成，从而增强Cu与载体的界面电子相互作用，提高Cu+活性中心的稳定性。其中，nd掺杂ZrO2负载的Cu催化剂表现出较高的CO2转化率和对甲醇的选择性等催化性能。各种表征（XRD， SEM，原位XPS， H2-TPR， CO2-TPD和H2-TPD）结果证实了nd掺杂在调节氧缺陷，电子结构和Cu在载体上的分布中的关键作用。本研究从支撑工程的角度揭示了Nd在构建高效cu基CO2加氢催化剂中的结构调控机制，为新型高性能催化材料的设计提供理论依据和实践指导。

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引用次数: 0

Catalyst development for the hydrogen to propylene oxide process with in-situ generated hydrogen peroxide and intensification in a trickle bed reactor 原位生成过氧化氢及滴流床强化氢制环氧丙烷催化剂的研制

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-22 DOI: 10.1016/j.apcata.2025.120756

Christoph Schmidt , Francesco Sandri , Alice Vidrequin , Jeremy Favier , Atte Aho , Sari Granroth , Mika Lastusaari , Tapio Salmi

Novel continuous propylene oxide production via in-situ generated hydrogen peroxide under mild liquid phase conditions was optimized by tailoring gold-palladium on titanium silicalite 1 (TS-1) catalysts and reaction parameters. AuPd alloy nanoparticles were deposited on two commercial TS-1 supports, with and without anatase impurities. On anatase-free TS-1, highly dispersed AuPd nanoparticles (6–10 nm) were formed, whereas in anatase-containing TS-1, metal precursors preferentially deposited on anatase, yielding larger nanoparticles after calcining. Ammonium hydroxide and water, water-only washing, and no washing were applied after synthesis, with water-only washing yielding smallest nanoparticles. Prolonged urea-deposition synthesis promoted metal redispersion, confirmed by material sampling during synthesis, and improved catalyst stability. In the combined direct synthesis of hydrogen peroxide and hydrogen peroxide to propylene oxide process (HPPO), smaller AuPd nanoparticles enhanced propylene oxide production but decreased propylene oxide selectivity by formation of propane and ring-opening products. Au-richer alloys improved propylene oxide selectivity but decreased propylene oxide productivity, while monometallic gold was inactive in the reaction system. Higher metal loadings increased propylene oxide productivity only for gold-richer alloys. Reaction parameter optimization identified that higher temperature and reduced liquid flow rate favored hydrogen peroxide conversion and ring-opening products formation, while shifting from propene-rich to oxygen-rich feed suppressed propane formation.

通过对钛硅石1 （TS-1）催化剂和反应参数的调整，优化了在温和液相条件下原位生成过氧化氢连续生产环氧丙烷的新工艺。AuPd合金纳米颗粒沉积在两个商用TS-1支架上，含有和不含锐钛矿杂质。在不含锐钛矿的TS-1中，形成了高度分散的纳米AuPd(6-10 nm)，而在含锐钛矿的TS-1中，金属前驱体优先沉积在锐钛矿上，煅烧后产生更大的纳米AuPd。合成后分别用氢氧化铵和水、纯水洗和不水洗，其中纯水洗产生的纳米颗粒最小。延长尿素沉积合成时间促进了金属的再分散，并提高了催化剂的稳定性。在双氧水和双氧水直接合成环氧丙烷（HPPO）工艺中，较小的AuPd纳米颗粒提高了环氧丙烷的产量，但通过丙烷和开环产物的形成降低了环氧丙烷的选择性。富金合金提高了环氧丙烷的选择性，但降低了环氧丙烷的产率，而单金属金在反应体系中无活性。较高的金属负荷只对含金较多的合金提高了环氧丙烷的生产率。反应参数优化发现，较高的温度和较低的液流量有利于过氧化氢的转化和开环产物的形成，而从富丙烯进料转向富氧进料抑制丙烷的形成。

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引用次数: 0

Novel advanced channel reactor for spatio-temporal activity and catalyst state correlations applied for the reduction of NO by CO over Pt/Al2O3 新型先进的通道反应器用于Pt/Al2O3上CO还原NO的时空活性和催化剂状态相关性

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-20 DOI: 10.1016/j.apcata.2025.120748

Thomas Häber , Sui Wan , Samuel Struzek , Camilo Cárdenas , Anna Zimina , Florian Maurer , Patrick Lott , Rainer Suntz , Jan-Dierk Grunwaldt , Olaf Deutschmann

The correlation of space- and time-resolved measurements of catalytic activity with catalyst state is an invaluable tool to advance the understanding and development of complex catalytic systems under conditions relevant to technical applications. Such an approach is employed here to investigate the catalytic deactivation in the reduction of NO by CO over Pt/Al₂O₃ on freshly reduced catalysts in a channel reactor and at concentrations typical for emission control. Planar laser-induced fluorescence (PLIF) is used to visualize the 2D concentration profiles and to derive space- and time-resolved NO conversion rates for different CO/NO ratios, temperatures and mass flow rates. The changes in catalytic activity are correlated with temporal and spatial changes in oxidation state determined by operando X-ray absorption spectroscopy (XAS) under the same conditions. The time scales of the changes in catalytic activity depend not only on the stoichiometry and temperature, but also on the position along the catalyst channel and differ significantly from the temporal changes of the oxidation state. The different time scales are discussed in the context of the known CO poisoning as well as the formation and storage of isocyanate on the support. Isocyanate formation temporarily counteracting CO poisoning could explain the differences in the observed time scales under different reaction conditions and at different locations on the catalyst.

在与技术应用相关的条件下，空间和时间分辨的催化活性测量与催化剂状态的相关性是促进对复杂催化系统的理解和发展的宝贵工具。本文采用这种方法，在通道反应器中，在典型的排放控制浓度下，研究了CO在Pt/Al2O3上新还原的催化剂上还原NO的催化失活。平面激光诱导荧光（PLIF）用于可视化二维浓度分布，并推导出不同CO/NO比、温度和质量流量下的空间和时间分辨NO转化率。在相同条件下，用x射线吸收光谱（XAS）测定氧化态的时空变化与催化活性的变化相关。催化活性变化的时间尺度不仅取决于化学计量和温度，还取决于催化剂通道上的位置，与氧化态的时间变化有很大的不同。在已知CO中毒以及异氰酸酯在载体上的形成和储存的背景下，讨论了不同的时间尺度。异氰酸酯的形成可以暂时抵消CO中毒，这可以解释不同反应条件下和催化剂上不同位置观察到的时间尺度的差异。

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引用次数: 0

In situ synthesis of stable and coking-resistant NiCo@La₂MoO₆ core-shell catalyst from perovskite precursor for dry reforming of methane 用钙钛矿前驱物原位合成稳定抗结焦NiCo@La₂MoO₆核壳催化剂用于甲烷干重整

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-20 DOI: 10.1016/j.apcata.2025.120755

Haoran Yu , Jucang Ke , Xuyingnan Tao , Feiyang Yu , Tingting Zhao , Ming Li , Haiqian Wang

Ni(Co)-based catalysts exhibit high activity for dry reforming of methane (DRM), but their rapid deactivation due to carbon deposition—especially at high metal loadings—remains a critical challenge. Herein, we report an in situ synthesis strategy for a coking-resistant NiCo@La₂MoO₆ core-shell catalyst derived from a perovskite precursor. The LaNi₀.₅Co₀.₄Mo₀.₁O₃ (LNCM1) precursor, synthesized via the sol−gel method, adopts a single-phase perovskite structure. During H₂ pretreatment and DRM reaction, in situ exsolution of Ni and Co atoms from the perovskite lattice occurs, accompanied by the formation of low-crystallinity La₂MoO₆. This process establishes a strong metal-support interaction (SMSI), enabling the self-assembly of a NiCo@La₂MoO₆ core-shell structure. The core-shell structure not only enhances catalytic activity but also suppresses carbon deposition, ensuring long-term stability. In contrast, the NiCo/La₂O₃ catalyst derived from the Mo-free LNC precursor—composed primarily of La(NiCo)O₃, La₂(NiCo)O₄, and La₂O₃—achieves high initial activity but rapidly deactivates due to severe carbon deposition. We propose that the binding strength and coverage of O* on the NiCo surface, modulated by Mo doping, play an essential role in determining the catalytic activity and coking resistance. However, there is a trade-off in the NiCo-O* interaction: while a strong interaction suppresses carbon deposition, it concurrently diminishes the activity. Incorporating Mo into La₂MoO₆ stabilized the high oxidation state of molybdenum, thereby optimizing the NiCo-O* interaction and enhancing catalytic performance in dry reforming of methane. This work advances the design of durable, coke-resistant NiCo-based DRM catalysts through tailored perovskite precursors.

Ni（Co）基催化剂在甲烷干重整（DRM）中表现出高活性，但由于碳沉积（特别是在高金属负载下）而导致的快速失活仍然是一个关键挑战。在这里，我们报道了一种由钙钛矿前驱体衍生的抗结焦NiCo@La₂MoO₆核壳催化剂的原位合成策略。的LaNi₀₄莫₀₅Co₀。溶胶-凝胶法合成的1₁O₃（LNCM1）前驱体采用单相钙钛矿结构。在H₂预处理和DRM反应过程中，Ni和Co原子从钙钛矿晶格中原位析出，形成低结晶度的La₂MoO₆。这一过程建立了强大的金属-支撑相互作用（SMSI），使NiCo@La₂MoO₆核壳结构能够自组装。核壳结构不仅提高了催化活性，而且抑制了碳沉积，保证了长期稳定性。相反，来自无mo LNC前驱体的NiCo/La₂O₃催化剂——主要由La(NiCo)O₃、La₂（NiCo）O₄和La₂O₃组成——具有很高的初始活性，但由于严重的碳沉积而迅速失活。我们认为，通过Mo掺杂调节的O*在NiCo表面的结合强度和覆盖范围是决定催化活性和抗结焦性的重要因素。然而，在NiCo-O*相互作用中存在一种权衡：当强相互作用抑制碳沉积时，它同时降低了活性。La₂MoO₆中加入Mo，稳定了钼的高氧化态，从而优化了NiCo-O*的相互作用，提高了甲烷干重整的催化性能。这项工作通过定制钙钛矿前驱体推进了耐用、耐焦的镍基DRM催化剂的设计。

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引用次数: 0

Covalent organic frameworks modified with imidazole units anchored Keggin-type heteropoly acids for production of furfural from xylose and corncob 以咪唑单元修饰的共价有机框架锚定keggin型杂多酸，用于木糖和玉米芯生产糠醛

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-19 DOI: 10.1016/j.apcata.2025.120754

Yunqing Liu , Xin Huang , Zhao Huang , Fang Su , Daiyu Song

A series of nitrogen-rich porous covalent imine network modified with imidazole units anchored Keggin-type H₃PW₁₂O₄₀ (PW-ICIN) were prepared via one-pot co-condensation strategy. The Keggin-type PW clusters can be in situ immobilized onto the ICIN support through physical confinement and hydrogen bonds. The synergistic catalytic effect between the N-rich units and the PW clusters of the catalyst was expected to boost catalytic activity. The catalytic performance of the PW-ICIN catalyst was systematically evaluated in the dehydration of xylose to furfural, with emphasis on the effects of reaction parameters, catalyst stability, and synergistic mechanisms. The catalytic activity of the PW-ICIN catalyst was higher than those of the commercial solid acids (e.g., Amberlyst-15 and HY zeolite) in production of furfural from xylose and corncob, respectively. The high yield of FF (52.7 % and 33.0 %) and TOF value (0.026 min^–1 and 0.054 min^–1) were obtained in the PW-ICIN-3-catalyzed xylose and corncob conversion, respectively, at 160 °C for 6 h. These advantages of appropriate acid properties, various N-rich units, and excellent porosity property of the PW-ICIN catalysts can significantly improve the catalytic activity. The reaction pathway and mechanism of production of FF from xylose have been reasonably speculated. The robust interaction between PW clusters and frameworks ensured the well reusability of PW-ICIN catalyst. This work aims to advance the rational design of COF-anchored heteropoly acids for sustainable biomass conversion.

采用一锅共缩聚法制备了咪唑基锚定keggin型H3PW12O40 （PW-ICIN）修饰的富氮多孔共价亚胺网络。keggin型PW簇可以通过物理约束和氢键原位固定在ICIN支架上。富n单元与PW簇之间的协同催化作用有望提高催化剂的催化活性。系统评价了PW-ICIN催化剂在木糖脱水制糠醛过程中的催化性能，重点考察了反应参数、催化剂稳定性和协同机理的影响。PW-ICIN催化剂在木糖和玉米芯制备糠醛过程中的催化活性分别高于商用固体酸（如Amberlyst-15和HY沸石）。pw - icin -3催化木糖和玉米芯转化，在160 °C、6 h下，FF的产率分别为52.7% %和33.0% %，TOF值分别为0.026 min-1和0.054 min-1。PW-ICIN催化剂具有适宜的酸性、丰富的富n单元和优异的孔隙性等优点，可显著提高催化剂的催化活性。对木糖生产FF的反应途径和机理进行了合理的推测。PW簇与框架之间的强相互作用保证了PW- icin催化剂的良好可重用性。本工作旨在促进cof锚定杂多酸的合理设计，以实现可持续的生物质转化。

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引用次数: 0

Harnessing high faradaic efficiency for n-butanol over Cu-cubic nanocrystals: New insights into CO2 reduction via GC-DFT and operando Raman spectroscopy 利用cu立方纳米晶体上正丁醇的高法拉第效率：通过GC-DFT和operando拉曼光谱对CO2减少的新见解

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-17 DOI: 10.1016/j.apcata.2025.120752

Esraa Kotob , Yousef A. Alsunni , Ahmed H. Biby , Omer Ahmed Taialla , Ijaz Hussain , Khalid Alhooshani , Saheed A. Ganiyu , Munzir H. Suliman , Muhammad Usman

n-Butanol is a valuable chemical commodity with a market price of approximately $1300/ton. It is usually made from propylene and syngas via the oxo process, but its reliance on fossil fuels is unsustainable. However, its direct electrochemical production from CO₂ in a single step remains a significant challenge due to high energy requirements and the need for specialized catalysts. In this study, we report a facile single-step electrochemical CO₂ conversion into n-butanol with high faradaic efficiency, bypassing the need for a cascade system. C-C coupling via dimerization into C₄ products (n-butanol) was facilitated on the size dependent Cu-cubic morphology (average 30 nm), having dominate crystal facet orientation {100}. The process achieved a Faradaic efficiency of 21 % for n-butanol and 54.4 % for ethylene at a current density of 750 mA cm⁻², demonstrating stability of over 25 h of operation. Mechanistic insights were gained through Grand Canonical Density Functional Theory (GC-DFT) calculations, which revealed the favored energetics for the C–C coupling pathway on Cu-cubic {100} rather than C₁ products desorption. Furthermore, operando Raman spectroscopy tracked the CH₂CHO* intermediate, which is important for the C-C coupling. This scalable flow cell system could offer a promising and sustainable route for industrial n-butanol production from CO₂.

正丁醇是一种有价值的化学商品，市场价格约为每吨1300美元。它通常由丙烯和合成气通过氧化过程制成，但它对化石燃料的依赖是不可持续的。然而，由于高能量需求和对专用催化剂的需求，单步从二氧化碳中直接电化学生产仍然是一个重大挑战。在这项研究中，我们报告了一种简单的一步电化学二氧化碳转化为正丁醇，具有很高的法拉第效率，绕过了级联系统的需要。通过二聚化成C4产物（正丁醇）的C-C偶联促进了尺寸相关的cu立方形貌（平均30 nm），具有主导晶面取向{100}。该工艺在电流密度为750 mA cm⁻²时，正丁醇的法拉第效率为21 %，乙烯的法拉第效率为54.4 %，稳定性超过25 h。通过大正则密度泛函理论（GC-DFT）计算，揭示了cu立方{100}上C-C耦合途径比C1产物脱附更有利的能量学。此外，operando拉曼光谱追踪了CH2CHO*中间体，这对C-C耦合很重要。这种可扩展的液流电池系统为从二氧化碳中提取正丁醇的工业生产提供了一条有前途和可持续的途径。

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引用次数: 0

Preface to the special issue in honor of Prof. Luca Lietti on his 65th birthday 为纪念卢卡·利蒂教授65岁生日而出版的特刊序言

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-17 DOI: 10.1016/j.apcata.2025.120753

Alessandra Beretta , Gianpiero Groppi , Matteo Maestri , Isabella Nova , Enrico Tronconi , Carlo Giorgio Visconti

引用次数: 0

Construction of MnOₓ catalysts rich in oxygen vacancies for highly selective oxidation of aromatic alcohols: Structure-activity relationship and mechanism study 高选择性氧化芳醇的富氧空位MnOₓ催化剂的构建：构效关系及机理研究

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-16 DOI: 10.1016/j.apcata.2025.120746

Huan Wang , Weitao Wang , Shuang Yue , Yang Liu , Jiaqi Zhu , Yiqian Yao , Zhen-Hong He

Developing highly efficient and stable non-precious metal oxide catalysts for selective oxidation reactions remains a key challenge in the field of heterogeneous catalysis. This study synthesized a series of manganese oxide catalysts with distinct structural characteristics by controlling the calcination temperature of the precursors. The results indicate that the calcination temperature significantly influences the catalyst's crystal structure, the distribution of manganese valence states, and the surface defect concentration. Among these, the manganese oxide calcined at 400 °C exhibits optimal catalytic performance due to its unique structural characteristics, which include residing at a phase transition boundary, a partial transition of Mn ion valence states, and the resulting abundance of surface oxygen vacancies. These structural features collectively regulate the catalyst's electronic structure, effectively promoting the adsorption, and activation of molecular oxygen. This generates superoxide radicals (·O₂^–) as key reactive oxygen species, thereby driving an efficient oxidation reaction cycle. This work elucidates the structure–activity relationship of manganese oxides in oxidative catalysis, providing important insights for designing metal oxide catalysts with specific surface defects and electronic properties.

开发高效、稳定的非贵金属氧化物催化剂用于选择性氧化反应仍然是多相催化领域的一个关键挑战。本研究通过控制前驱体的煅烧温度，合成了一系列具有不同结构特征的氧化锰催化剂。结果表明，煅烧温度对催化剂的晶体结构、锰价态分布和表面缺陷浓度有显著影响。其中，400°C煅烧的氧化锰由于其独特的结构特征，包括位于相变边界，Mn离子价态的部分转变，以及由此产生的丰富的表面氧空位，表现出最佳的催化性能。这些结构特征共同调节了催化剂的电子结构，有效地促进了分子氧的吸附和活化。这产生超氧自由基（·O2 -）作为关键的活性氧，从而驱动一个有效的氧化反应循环。这项工作阐明了锰氧化物在氧化催化中的构效关系，为设计具有特定表面缺陷和电子性能的金属氧化物催化剂提供了重要的见解。

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引用次数: 0

Sustainable chemical recycling of PET via methanolysis over engineered hydroxyapatite nanorod catalysts 工程羟基磷灰石纳米棒催化剂甲醇分解PET的可持续化学回收

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-16 DOI: 10.1016/j.apcata.2025.120751

Yu Yang , Qingmei Ge , Nan Jiang , Hongxiu Zhao , Yin-Hui Huang , Hang Cong , Song Yang , Wenfeng Zhao

The disposal of waste plastics, particularly polyethylene terephthalate (PET), is a growing environmental issue, with PET accounting for a significant portion of global plastic waste. This work presents an efficient catalytic strategy for upcycling PET to high-value dimethyl terephthalate (DMT) using engineered hydroxyapatite (HAP) as a solid catalyst. HAP was prepared and characterized under different calcination conditions, resulting in rod-like porous structures with mesoporous features. The HAP catalyst calcined at 700 °C exhibited excellent catalytic activity for the methanolysis of PET, achieving 100 % PET conversion and more than 90 % DMT yield at 180 °C within 2 h. Notably, HAP showed good reusability, maintaining its catalytic performance over at least four cycles without significant deactivation. The mechanism of the HAP-catalyzed methanolysis of PET was studied via SEM and ³¹P solid-state NMR, revealing its role in promoting ester bond cleavage through both Lewis and Brønsted acid sites. This approach provides an efficient pathway for PET recycling, offering a sustainable solution to the growing problem of plastic waste.

废塑料的处理，特别是聚对苯二甲酸乙二醇酯（PET），是一个日益严重的环境问题，PET占全球塑料废物的很大一部分。本研究提出了一种利用工程羟基磷灰石（HAP）作为固体催化剂将PET升级为高价值对苯二甲酸二甲酯（DMT）的有效催化策略。在不同的煅烧条件下制备了HAP并对其进行了表征，得到了具有介孔特征的棒状多孔结构。在700℃下煅烧的HAP催化剂对PET的甲醇分解表现出优异的催化活性，在180℃下，2 h内PET转化率达到100% %，DMT产率达到90% %以上。值得注意的是，HAP表现出良好的可重复使用性，在至少四个循环中保持其催化性能而没有明显的失活。通过SEM和31P固体核磁共振研究了hap催化PET甲醇分解的机理，揭示了其通过Lewis和Brønsted酸位点促进酯键裂解的作用。这种方法为PET回收提供了有效途径，为日益严重的塑料废物问题提供了可持续的解决方案。

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引用次数: 0

Rice husk derived biochar as support for Ni based catalysts in CO2 methanation: A study on biochar activation 稻壳生物炭作为Ni基催化剂在CO2甲烷化中的载体：生物炭活化研究

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-12-14 DOI: 10.1016/j.apcata.2025.120750

Giulia Da Pian , Rachele Braido , Ivo Alxneit , Giuseppe Cruciani , Federica Menegazzo , Michela Signoretto

Waste derived biochars are becoming fundamental carbonaceous sources to be used as support in catalysis, especially after activation to improve their features. CO₂ methanation is a strategic process for energy transition. However, it requires better selectivity and economic feasibility. This can be done by acting on the catalytic system. In this article, a biochar from rice husk biomass was obtained by pyrolysis and activated in two different physical ways (water vapor and CO₂). The activated biochars were used to prepare CO₂ methanation catalysts with Ni 10 wt%. The starting biochars and final catalysts were characterized to investigate their morphological, physical and chemical features through various techniques to elucidate activation treatment effects on the ultimate catalyst performance. The best catalyst Ni/RHCO₂ presented good stability over 20 h of test and optimal selectivity values (>90 %), probably because of the better biochar features provided by CO₂ activation such as porosity, crystallinity, and stronger Ni-biochar interactions.

废物生物炭正成为催化的基本碳质来源，特别是在活化后，以改善其特性。二氧化碳甲烷化是能源转型的战略过程。然而，它需要更好的选择性和经济可行性。这可以通过作用于催化体系来实现。本文以稻壳生物质为原料，通过热解制备生物炭，并以水蒸气和CO2两种不同的物理方式进行活化。利用活性炭制备了含ni10 wt%的CO2甲烷化催化剂。通过对起始生物炭和最终催化剂的形态、物理和化学特征的研究，阐明活化处理对催化剂最终性能的影响。最佳催化剂Ni/RHCO2在20 h以上表现出良好的稳定性和最佳选择性值（>90 %），这可能是因为CO2活化提供了更好的生物炭特性，如孔隙度、结晶度和更强的Ni-生物炭相互作用。

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引用次数: 0