Catalysis Letters最新文献_第8页

Growth-associated and Non-growth-associated Bioethanol Production Kinetics from Nanoadsorbent-Detoxified Pretreated Hydrolysate 纳米吸附剂解毒预处理水解液的生长相关和非生长相关生物乙醇生产动力学

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-21 DOI: 10.1007/s10562-024-04868-8

Adeniyi P. Adebule, Isaac A. Sanusi, Gueguim E. B. Kana

Lignocellulosic-based (LCB) bioethanol production is challenged by the presence of inhibitory compounds in pretreated LCB hydrolysates limiting productivity. The negative impact of these inhibitory compounds on LCB bioethanol production kinetics remain understudied. Hence, this study modelled the kinetics of bioethanol fermentation using nanoadsorbent-detoxified potato peel waste (PPW) hydrolysate. Four different fermentation processes under both separate hydrolysis and fermentation (SHF) and simultaneous saccharification and fermentation (SSF) conditions, including A (SHF with non-detoxified hydrolysate), B (SSF with non-detoxified hydrolysate), C (SHF with detoxified hydrolysate), and D (SSF with detoxified hydrolysate) were evaluated for bioethanol productivity. Higher productivity of 1.23 and 1.16-fold increments were recorded for fermentation processes C and D. Thereafter, the experimental data for cell growth, bioethanol production and substrate utilisation were well-fitted by the logistic function, modified Gompertz, and Luedeking-Piret models respectively. Moreover, the obtained root-mean-square error (RMSE) and mean square error (MSE) were low, while the accuracy factor (AF), bias factor (BF), slope and regression coefficient (R²) were close to 1. The bioethanol production processes were largely growth-associated (α) as α values (g ethanol/g substrate) were higher than β values (g ethanol/g substrate/h). The models were effectively implemented, demonstrating their usefulness to elucidate bioethanol productivity kinetics for improved process design and the development of large-scale bioethanol production.

Graphical Abstract

基于木质纤维素（LCB）的生物乙醇生产受到预处理的LCB水解物中存在抑制化合物的挑战，限制了生产效率。这些抑制化合物对LCB生物乙醇生产动力学的负面影响仍未得到充分研究。因此，本研究模拟了利用纳米吸附剂解毒马铃薯皮废物（PPW）水解物发酵生物乙醇的动力学。在单独水解和发酵（SHF）和同时糖化和发酵（SSF）条件下，评估了四种不同的发酵工艺，包括A（含非解毒水解液的SHF）、B（含非解毒水解液的SSF）、C（含解毒水解液的SHF）和D（含解毒水解液的SSF）的生物乙醇产量。发酵过程C和d的产量分别增加了1.23倍和1.16倍。随后，细胞生长、生物乙醇产量和底物利用率的实验数据分别通过logistic函数、改进的Gompertz和Luedeking-Piret模型得到了很好的拟合。得到的均方根误差（RMSE）和均方误差（MSE）较低，精度因子（AF）、偏倚因子（BF）、斜率和回归系数（R2）均接近1。由于α值（g乙醇/g底物）高于β值（g乙醇/g底物/h），生物乙醇生产过程主要与生长相关（α）。这些模型有效地实现了，证明了它们对阐明生物乙醇产率动力学的有用性，有助于改进工艺设计和大规模生物乙醇生产的发展。图形抽象

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引用次数: 0

Enhanced Photocatalytic Performance of B/P Doped g-C3N4 for Pollutant Degradation: First-Principles Calculation Study B/P掺杂g-C3N4对污染物降解光催化性能的增强：第一性原理计算研究

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-21 DOI: 10.1007/s10562-025-04937-6

Zimo Wang, Jian Xiong, Xiaoling He, Bitao Xiong, Xing’ao Li

Graphitic carbon nitride (g-C₃N₄) is a visible light catalyst with considerable potential, offering broad application prospects in fields such as pollutant decomposition. In this study, we systematically investigated the geometric, electronic, and optical properties of B-doped, P-doped, and B/P co-doped g-C₃N₄ using first-principles methods. We also examined the adsorption effects of g-C₃N₄ on emerging oxidants, periodate (PI) and Peroxymonosulfate (PMS). The results showed that B/P co-doping significantly narrowed the band gap of g-C₃N₄ to 0.39 eV, transforming it into a direct band gap structure. Additionally, the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) exhibit enhanced delocalization, particularly over the bridging N1 atoms, which improved carrier mobility. Compared to pristine g-C₃N₄, the optical absorption demonstrated a more favorable response to visible light. Notably, the B/P co-doping system significantly increased the adsorption capacity of g-C₃N₄ for PI and PMS, promoting the generation of reactive species such as singlet oxygen (¹O₂), sulfate radicals (SO·₄⁻), and hydroxyl radicals (·OH), providing a favorable pathway for the degradation of pollutants in water. In summary, B/P co-doping significantly enhances the photocatalytic performance of g-C₃N₄, establishing it as a highly efficient, eco-friendly, and cost-effective metal-free photocatalyst with great potential for advanced oxidation processes under visible light in wastewater treatment.

Graphical Abstract

石墨氮化碳（g-C3N4）是一种具有相当潜力的可见光催化剂，在污染物分解等领域具有广阔的应用前景。在这项研究中，我们使用第一性原理方法系统地研究了B掺杂、P掺杂和B/P共掺杂g-C3N4的几何、电子和光学性质。我们还研究了g-C3N4对新兴氧化剂高碘酸盐（PI）和过氧单硫酸盐（PMS）的吸附效果。结果表明，B/P共掺杂使g-C3N4的带隙明显缩小至0.39 eV，使其转变为直接带隙结构。此外，最高占据分子轨道（HOMO）和最低未占据分子轨道（LUMO）表现出增强的离域性，特别是在桥接N1原子上，这提高了载流子的迁移率。与原始的g-C3N4相比，光学吸收表现出对可见光更有利的响应。值得注意的是，B/P共掺杂体系显著提高了g-C3N4对PI和PMS的吸附能力，促进了单线态氧（1O2）、硫酸盐自由基（SO·4−）和羟基自由基（·OH）等活性物质的生成，为降解水中污染物提供了有利的途径。综上所述，B/P共掺杂显著提高了g-C3N4的光催化性能，使其成为一种高效、环保、低成本的无金属光催化剂，在废水处理中具有很大的应用潜力。图形抽象

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引用次数: 0

Unveiling Reduction of NH3 Production in Pd-Based Three-Way Catalyst Modified by Ru Ru改性钯基三元催化剂中NH3产率降低的研究

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-21 DOI: 10.1007/s10562-024-04923-4

Xi Liu, Xiaoning Ren, Yuankai Shao, Anqi Dong, Chunqing Yang, Kaixiang Li, Bingjie Zhou, Hanming Wu, Zhenguo Li

Three-way catalyst (TWC) stands as the state-of-the-art technology for controlling emissions in natural gas vehicles, but its utilization can generate NH₃ by-product. This study proposed a novel strategy for reducing NH₃ emissions during three-way catalytic reaction process of Pd-based catalysts by adding Ru. Catalysts Pd/LA + Si, Pd/LA + Ru/CZLN, and Pd/LA + CZLN were fabricated through incipient wetness impregnation and mechanical ball-milling methods. Testing under simulated exhaust conditions showed that Pd/LA + Si produced high NH₃ levels, while Ru/CZLN addition significantly reduced NH₃ emissions from 330 to 20 ppm. Conversely, the addition of CZLN facilitated steam reforming and water–gas shift reactions, generating more H₂ for NO reduction, which led to an increase in NH₃ emissions. Experimental evidence confirmed that Ru/CZLN could effectively decompose NH₃, which was produced over Pd/LA, into N₂ and H₂, thereby significantly reducing NH₃ emissions. This study provides a promising approach for developing TWC with low NH₃ emissions for natural gas vehicles.

Graphical Abstract

三元催化剂（Three-way catalyst， TWC）是控制天然气汽车排放的最先进技术，但其使用会产生NH3副产物。本研究提出了一种通过添加Ru来降低钯基催化剂三元催化反应过程中NH3排放的新策略。采用初湿浸渍法和机械球磨法制备了Pd/LA + Si、Pd/LA + Ru/CZLN和Pd/LA + CZLN催化剂。在模拟排气条件下的测试表明，Pd/LA + Si产生了高水平的NH3，而Ru/CZLN的添加显著降低了NH3的排放量，从330 ppm降至20 ppm。相反，CZLN的加入促进了蒸汽重整和水煤气转移反应，产生更多的H2来还原NO，导致NH3排放量增加。实验证实Ru/CZLN可以有效地将Pd/LA上产生的NH3分解成N2和H2，从而显著减少NH3的排放。该研究为开发天然气汽车低NH3排放TWC提供了一条有希望的途径。图形抽象

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引用次数: 0

Analysis of Deactivation Causes and Regeneration Study of RuO2 /TiO2 in Industrial Catalytic Wet Oxidation Process RuO2 /TiO2工业湿法催化氧化失活原因分析及再生研究

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-18 DOI: 10.1007/s10562-024-04915-4

Tong Cui, Wenjing Sun, Danyang Yu, Weiling Piao, Huangzhao Wei, Xu Yang, Chenglin Sun

RuO₂ /TiO₂, as the main catalyst in wet catalytic oxidation, faces the problem of catalyst deactivation while treating high concentration organic wastewater efficiently and without pollution. There have been many studies on catalyst deactivation and regeneration, but most of them are based on laboratory simulation environment. Due to the complexity of industrial environments, the causes of industrial catalyst deactivation are still unclear, while there are very few studies on regeneration. Herein, we characterized industrially used catalysts and found that the causes of catalyst deactivation can be attributed to two reasons, namely, the change of carrier crystal shape and carbon accumulation. Thermal regeneration to address the carbon accumulation problem restores some of the physicochemical properties of the used catalysts, however, thermal regeneration cannot restore the catalyst support phase from rutile back to anatase, resulting in the inability to restore catalyst activity. Therefore, the catalyst was regenerated by the method of direct addition of active components, and the catalyst activity was basically restored when the Ru mass fraction was 0.5%. Moreover, the method of directly adding active components has the advantages of simplicity and no energy consumption, which is easy to be utilized in the industrial production process.

Graphical Abstract

RuO2 /TiO2作为湿式催化氧化中的主要催化剂，在高效、无污染地处理高浓度有机废水的同时，面临着催化剂失活的问题。关于催化剂失活与再生的研究很多，但大多是基于实验室模拟环境。由于工业环境的复杂性，工业催化剂失活的原因尚不清楚，而对再生的研究很少。本文对工业上使用的催化剂进行了表征，发现催化剂失活的原因可以归结为两个原因，即载体晶体形状的改变和碳的积累。热再生解决了碳积累问题，恢复了催化剂的部分理化性质，但热再生不能将催化剂的支撑相从金红石还原为锐钛矿，导致催化剂活性无法恢复。因此，采用直接添加活性组分的方法对催化剂进行再生，当Ru质量分数为0.5%时，催化剂活性基本恢复。而且，直接添加活性成分的方法具有简单、不消耗能源的优点，易于在工业生产过程中加以利用。图形抽象

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引用次数: 0

Manganese Ferrite Supported on Activated Alumina Beads for Activation of Periodate Towards Efficient Degradation of Organic Dye Pollutants 活性氧化铝珠载铁酸锰活化高碘酸盐高效降解有机染料污染物

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-18 DOI: 10.1007/s10562-024-04919-0

Yawei Shi, Chang Ma, Yumei Xing, Ya Sun, Guanghui Ding

Manganese ferrite (MnFe₂O₄) supported on activated alumina beads (MFO-AABs) was synthesized by solvothermal method and used to activate periodate (PI) to degrade crystal violet (CV) and other organic dye pollutants. Under the optimum conditions (MFO-AABs dosage of 10 beads and PI dosage of 0.4 g/L), the removal efficiency of 10 mg/L CV reached 98.3% in 120 min. This surpassed the sum of removal efficiencies when MFO-AABs and PI presented respectively, indicating that MFO-AABs and PI worked synergistically. The removal efficiency of CV was almost unaffected in the presence of SO₄²⁻(aq.) while slightly inhibited by Cl⁻(aq.), HCO₃⁻(aq.) or HPO₄²⁻(aq.). The effect of initial pH was studied in the range of 3–9, showing that the removal performance of CV was better under acidic and neutral conditions. Reusability tests showed that the removal efficiency of CV declined slightly after MFO-AABs was reused for 4 times, which was attributed to the accumulation of degradation products on the catalyst. Through calcination to remove these adsorbed degradation products, the catalytic ability could be recovered. Quenching experiments showed that ¹O₂ played a major role in the reaction process. The contribution of non-radical electron transfer was ruled out by a series of electrochemical tests. In addition, IO₄⁻(aq.) was stoichiometrically converted to IO₃⁻(aq.) without producing potentially toxic iodine species such as I⁻(aq.), I₂/I₃⁻(aq.) and HOI. Combining liquid chromatography-mass spectrometry (LC-MS) and density functional theory (DFT) calculations, the possible degradation pathway of CV was proposed with 12 degradation products. Finally, the analysis of potential toxicity was carried out by theoretical calculations as well as experiments with Vigna radiata, revealing the decreased potential toxicity after the degradation process.

Graphical Abstract

采用溶剂热法合成了负载在活性氧化铝珠（MFO-AABs）上的铁酸锰（MnFe2O4），并将其用于活化高酸盐（PI）降解结晶紫（CV）等有机染料污染物。在最佳条件下（MFO-AABs投加量为10微珠，PI投加量为0.4 g/L）， 120 min对10 mg/L CV的去除率可达98.3%。这超过了MFO-AABs和PI分别存在时的去除效率之和，表明MFO-AABs与PI协同作用。SO42−(aq.)对CV的去除率几乎没有影响，Cl−(aq.)、HCO3−(aq.)和HPO42−(aq.)对CV的去除率有轻微的抑制作用。研究了初始pH值在3 ~ 9范围内的影响，结果表明，酸性和中性条件下对CV的去除效果较好。重复使用试验表明，MFO-AABs重复使用4次后，CV的去除率略有下降，这是由于降解产物在催化剂上积累所致。通过煅烧去除这些吸附的降解产物，可以恢复催化能力。淬火实验表明，1O2在反应过程中起主要作用。通过一系列电化学试验，排除了非自由基电子转移的影响。此外，IO4−(aq.)被化学计量转化为IO3−(aq.)，而不会产生潜在的有毒碘物质，如I−(aq.), I2/I3−(aq.)和HOI。结合液相色谱-质谱（LC-MS）和密度泛函理论（DFT）计算，提出了12种降解产物对CV可能的降解途径。最后，通过理论计算和Vigna radiata实验进行了潜在毒性分析，揭示了降解过程后潜在毒性的降低。图形抽象

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引用次数: 0

Ascorbic Acid Enhanced the Performance of Pd/ZrO2 for Efficient Hydrogenation of Phenol in Aqueous Phase 抗坏血酸增强了Pd/ZrO2水溶液中苯酚的高效加氢性能

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-18 DOI: 10.1007/s10562-024-04917-2

Yu Wang, Xin Zhang, Shiling Fan, Zhiying Wang, Hao Li

The design of high-performance, mild-condition HDO catalysts is a crucial step in the high-value utilization of the conversion of phenol to cyclohexanone. In this paper, the effect of modifier on the catalyst activity was investigated by surface modification of ZrO₂ support by ascorbic acid (AA). The role of water in the reaction solvent was also explored. The results showed that ascorbic acid can etch the surface lattice of the support and generate reactive oxygen vacancies; the OH group can act as an acid site and stabilise the C = O group in cyclohexanone through “acid-base interaction”, thus inhibiting further hydrogenation of cyclohexanone. In addition, the transfer of hydrogen in the aqueous phase facilitated the isomerisation of the enol to cyclohexanone and inhibited the occurrence of side reactions. The Pd/ZrO₂ + AA catalyst resulted in a phenol conversion of 58.3% and a cyclohexanone selectivity of 85.7% in 2 h at a water/methanol volume ratio of 2/8. Moreover, the catalyst showed good stability, with no significant decrease in phenol conversion and the selectivity of cyclohexanone remaining at 80.6% after four cycles. This study aimed to provide a new avenue for the high-value utilization of phenol by modulating the catalyst preparation and optimising the reaction system.

Graphical abstract

设计高性能、温和条件的HDO催化剂是实现苯酚制环己酮高值利用的关键一步。本文采用抗坏血酸（AA）对ZrO2载体进行表面改性，研究了改性剂对催化剂活性的影响。探讨了水在反应溶剂中的作用。结果表明：抗坏血酸能腐蚀载体表面晶格，产生活性氧空位；羟基可以作为酸位，通过“酸碱相互作用”稳定环己酮中的C = O基团，从而抑制环己酮的进一步加氢。此外，水相中氢的转移促进了烯醇异构化成环己酮，抑制了副反应的发生。在水/甲醇体积比为2/8的条件下，Pd/ZrO2 + AA催化剂在2 h内苯酚转化率为58.3%，环己酮选择性为85.7%。催化剂稳定性好，4次循环后苯酚转化率无明显下降，环己酮的选择性保持在80.6%。本研究旨在通过调整催化剂制备和优化反应体系，为苯酚的高价值利用提供一条新的途径。图形抽象

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引用次数: 0

DFT Study on S-Scheme g-C3N4/g-C3N4(P) Heterostructure Photocatalyst in Hydrogen Production Process by Photocatalytic Water Splitting S-Scheme g-C3N4/g-C3N4(P)异质结构光催化剂在光催化水裂解制氢过程中的DFT研究

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-18 DOI: 10.1007/s10562-024-04929-y

Houmei Dai, Xin Li, Yanglai Hou, Dongliang Wang, Ran Wei

The recombination of electrons and holes in the semiconductor photocatalyst seriously affects the hydrogen production efficiency in photocatalytic water splitting. The appearance of S-scheme heterojunction can greatly reduce the recombination rate. In order to enrich this type of photocatalyst, the performance of metal-free g-C₃N₄/g-C₃N₄(P) heterostructure is studied theoretically. The negative adhesion energy proves the stability of the heterostructure. Research on PDOS, projected band structures, charge transfer, band edge positions and photocatalytic mechanism shows more clearly and comprehensively that this g-C₃N₄/g-C₃N₄(P) heterostructure is S-scheme with high redox ability. The near-zero ∆G_H* of free energy change in HER process indicates that this g-C₃N₄/g-C₃N₄(P) heterostructure should have good HER performance. This work enriches the photocatalyst types and provides a theoretical support for the experimental study of corresponding photocatalysts.

Graphical Abstract

半导体光催化剂中电子与空穴的复合严重影响光催化水分解产氢效率。s型异质结的出现可以大大降低复合速率。为了丰富这类光催化剂，从理论上研究了无金属g-C3N4/g-C3N4(P)异质结构的性能。负的附着能证明了异质结构的稳定性。通过对PDOS、投影带结构、电荷转移、带边位置和光催化机理的研究，更清晰、全面地证明了g-C3N4/g-C3N4(P)异质结构为具有高氧化还原能力的s型方案。HER过程中自由能变化的∆GH*接近于零，说明该g-C3N4/g-C3N4(P)异质结构具有良好的HER性能。这一工作丰富了光催化剂的种类，为相应光催化剂的实验研究提供了理论支持。图形抽象

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引用次数: 0

Ethanol-Based Transesterification of Rapeseed Oil with CaO Catalyst: Process Optimization and Validation Using Microalgal Lipids 微藻脂催化乙醇基菜籽油酯交换工艺优化与验证

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-18 DOI: 10.1007/s10562-024-04921-6

Gabriela F. Ferreira, Luisa F. Ríos Pinto, Rubens Maciel Filho, Leonardo V. Fregolente, James Hayward, Jonathan K. Bartley

Microalgal oil has been increasingly studied as a feedstock for biodiesel production through transesterification reactions using heterogeneous catalysts. This route offers several benefits, including catalyst reuse, ease of separation, and improved safety, while addressing environmental and technical issues associated with using homogeneous acids and bases. Most studies use methanol for the transesterification, and few studies have investigated the transesterification of microalgal oil using ethanol. Beyond the environmental benefits of microalgae compared to plant-based biomass, replacing methanol with bioethanol is advantageous due to its lower cost and reduced toxicity. If the emulsion issue between the produced biodiesel and ethanol is resolved, ethanol could be a more environmentally friendly alternative for green fuel production. This study evaluated various metal oxides as catalysts for the transesterification of rapeseed oil using ethanol as both reagent and solvent to improve miscibility. From catalyst screening, CaO showed the highest fatty acid ethyl esters yield and this catalyst was then tested at different reaction times in two systems (round-bottom flask and autoclave reactor) for the transesterification of both rapeseed and microalgal (Scenedesmus sp.) oil. The highest reaction yield was 86.0% for rapeseed oil and 81.3% for microalgal oil using 114:1 ethanol: oil molar ratio with CaO in an autoclave reactor. This work addresses the limited studies on ethanol in microalgal oil transesterification, demonstrating the effectiveness of CaO as a catalyst. It highlights the potential of ethanol as a greener, cost-effective alternative to methanol for biodiesel production.

Graphical Abstract

微藻油作为生物柴油原料，利用多相催化剂进行酯交换反应已得到越来越多的研究。该路线具有多种优势，包括催化剂可重复使用、易于分离、安全性提高，同时解决了使用均相酸和碱所带来的环境和技术问题。大多数研究使用甲醇进行酯交换，很少有研究使用乙醇进行微藻油的酯交换。除了与植物基生物质相比，微藻的环境效益外，用生物乙醇替代甲醇的优势在于其成本更低，毒性更低。如果所生产的生物柴油和乙醇之间的乳化问题得到解决，乙醇可能是一种更环保的绿色燃料生产替代品。以乙醇为溶剂和试剂，考察了不同金属氧化物对菜籽油酯交换反应的催化作用。从催化剂筛选中，CaO的脂肪酸乙酯收率最高，并在两种体系（圆底烧瓶和高压釜反应器）中对该催化剂进行了不同反应时间的测试，用于油菜籽和微藻油的酯交换。在高压釜反应器中，乙醇：油摩尔比为114:1时，菜籽油和微藻油的反应收率最高，分别为86.0%和81.3%。这项工作解决了微藻油酯交换中乙醇的有限研究，证明了CaO作为催化剂的有效性。它强调了乙醇作为一种更环保、更具成本效益的替代甲醇生产生物柴油的潜力。图形抽象

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引用次数: 0

Design, Synthesis, Characterization and Catalytic Activity of Chromium Oxide Nanoparticles Immobilized on Layered Double Hydroxide as Competent Nanocatalyst 层状双氢氧化物固定氧化铬纳米颗粒的设计、合成、表征及催化活性研究

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-18 DOI: 10.1007/s10562-024-04926-1

Jagat Singh Kirar

Transition metals are commonly used in the oxidation of cyclohexane, but their harsh reaction conditions and lack of efficiency make further use challenging. In this study, we prepared chromium nanoparticles supported on layered double hydroxide abbreviated as Cr₂O₃/LDH. The physiochemical properties of synthesized nanocatalysts were extensively studied using FTIR, XRD, SEM, EDX, TEM, ICP-AES, and XPS technique. The synthesized Cr₂O₃/LDH nanocatalyst was used to the liquid phase selective oxidation of cyclohexane under solvent-free condition. The characterization result indicates that the Cr₂O₃-NPs were uniformly dispersed on the surface of LDH. The Cr₂O₃-NPs alone have relatively low catalytic activity, while LDH has no catalytic activity. However, the Cr₂O₃-NPs/LDH hybrid significantly increases both the conversion and selectivity. A maximum conversion of 34.73% cyclohexane and 97.85% selectivity to KA oil obtained over the Cr₂O₃/LDH nanocatalyst. Furthermore, the leaching test showed that the Cr₂O₃/LDH nanocatalyst was heterogeneous and could be recycled at least six cycles without significant loss in catalytic efficiency.

Graphical Abstract

过渡金属通常用于环己烷的氧化，但其恶劣的反应条件和缺乏效率使得进一步使用具有挑战性。在本研究中，我们制备了层状双氢氧化物（简称Cr2O3/LDH）负载的纳米铬。采用FTIR、XRD、SEM、EDX、TEM、ICP-AES、XPS等技术对合成的纳米催化剂的理化性质进行了研究。将合成的Cr2O3/LDH纳米催化剂用于环己烷在无溶剂条件下的液相选择性氧化。表征结果表明，Cr2O3-NPs均匀分布在LDH表面。单独的Cr2O3-NPs具有较低的催化活性，而LDH没有催化活性。然而，Cr2O3-NPs/LDH杂化物显著提高了转化率和选择性。在Cr2O3/LDH纳米催化剂上，环己烷转化率为34.73%，KA油选择性为97.85%。此外，浸出试验表明，Cr2O3/LDH纳米催化剂是多相的，可以循环使用至少6次，而催化效率没有明显损失。图形抽象

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引用次数: 0

FeOOH-NiV LDH Heterostructure as Efficient Electrocatalyst for Oxygen Evolution Reaction feoh - niv LDH异质结构作为析氧反应的高效电催化剂

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2025-01-18 DOI: 10.1007/s10562-024-04894-6

Shengwang Liu, Shixue Song, Yi Feng

The oxygen evolution reaction (OER) with complex 4-electron transfer is a critical issue limiting the efficiency of electrolytic hydrogen production. Therefore, to develop efficient OER electrocatalysts for water splitting was necessary. Given the abundant unoccupied 3d orbitals of high-valent vanadium ions and the three-dimensional structure of nickel foam substrates, this study successfully fabricate hydroxy-iron oxide (FeOOH) modified nickel vanadium layered double hydroxide (NiV LDH) nanosheets array heterostructure electrocatalysts through surface modification method. By coupling FeOOH with NiV LDH, the electron structure between Fe, Ni, V, and O was finely regulated. Thanks to the strong electronic interactions at the heterostructure interface, the prepared heterostructure electrocatalysts exhibit outstanding electrocatalytic OER performance in 1 M KOH electrolyte. The heterostructure electrocatalyst demonstrated overpotentials of only 212, 252, and 279 mV at current densities of 10, 50, and 100 mA·cm⁻², respectively, and a Tafel slope of only 71.37 mV·dec⁻¹. This study provided a new strategy for developing efficient new OER heterostructure catalysts.

Graphical Abstract

具有复杂4电子转移的析氧反应（OER）是制约电解制氢效率的关键问题。因此，开发高效的OER水裂解电催化剂是必要的。考虑到高价钒离子丰富的未占据三维轨道和泡沫镍基底的三维结构，本研究通过表面修饰方法成功制备了羟基氧化铁（FeOOH）修饰的镍钒层状双氢氧化物（NiV LDH）纳米片阵列异质结构电催化剂。通过FeOOH与NiV LDH的耦合，Fe、Ni、V、O之间的电子结构得到了很好的调控。由于异质结构界面处存在较强的电子相互作用，制备的异质结构电催化剂在1 M KOH电解质中表现出优异的电催化OER性能。在电流密度为10、50和100 mA·cm−2时，异质结构电催化剂的过电位分别为212、252和279 mV， Tafel斜率仅为71.37 mV·dec−1。本研究为开发高效OER异质结构催化剂提供了新的思路。图形抽象

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