Catalysis Science & Technology最新文献_第5页

Multivariate analysis coupled to infrared spectroscopy unravels the diversity of adsorption sites and strengths of a zeolite surface 多变量分析与红外光谱相结合揭示了沸石表面吸附位点和强度的多样性

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-04-09 DOI: 10.1039/d6cy00101g

Reda Aboulayt , Eleonora Vottero , Alexandre Vimont , Philippe Bazin , Emily Bloch , Sandrine Bourrelly , Sylvie Maury , Céline Chizallet , Arnaud Travert

Quantifying adsorption thermodynamics on heterogeneous catalysts remains challenging because macroscopic techniques yield averaged parameters, while vibrational spectra often contain strongly overlapping contributions from multiple adsorbed species. Here we introduce an infrared (IR)-chemometric framework that extracts site-specific adsorption thermodynamics directly from experimental IR isotherms and we benchmark it against independent microcalorimetry and density functional theory (DFT) calculations. Difference IR spectra recorded for isobutanol adsorption on H-ZSM-5 (MFI) were analysed by principal component analysis and multivariate curve resolution (MCR-ALS) under soft constraints (monotonic concentration profiles, spectral normalisation), and further refined using a hard–soft strategy in which concentration profiles are constrained by an adsorption model. The analysis reveals three adsorption modes associated with bridging Brønsted OH groups, extra-framework Al–OH species, and silanols, providing representative pure-component spectra and site-resolved adsorption isotherms. The thermodynamic trends and site hierarchy obtained from IR–MCR-ALS are consistent with independent microcalorimetry measurements and density functional theory calculations, validating the approach. More broadly, IR–MCR-ALS offers a transferable route to quantitative, site-resolved adsorption thermodynamics in complex catalysts.

量化多相催化剂的吸附热力学仍然具有挑战性，因为宏观技术只能得到平均参数，而振动光谱通常包含多种吸附物质的强烈重叠贡献。在这里，我们介绍了一个红外(IR)-化学计量框架，它直接从实验红外等温线中提取特定位置的吸附热力学，并将其与独立的微热量法和密度泛函理论（DFT）计算相比较。采用主成分分析和多元曲线分辨率（MCR-ALS）对H-ZSM-5 （MFI）吸附异丁醇的不同红外光谱进行分析，并在软约束条件下（单调浓度曲线、光谱标准化），进一步采用吸附模型约束浓度曲线的软硬策略进行细化。分析揭示了三种与桥接Brønsted OH基团、框架外Al-OH基团和硅烷醇相关的吸附模式，提供了具有代表性的纯组分光谱和位置分辨吸附等温线。由IR-MCR-ALS得到的热力学趋势和位点层次与独立的微热测量和密度泛函理论计算一致，验证了该方法的有效性。更广泛地说，IR-MCR-ALS提供了一种可转移的路线，用于复杂催化剂的定量，位点分解吸附热力学。

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引用次数: 0

Catalyst development for the efficient synthesis of pentanediols via the selective hydrogenation of biomass-based furfural and its derivatives 生物质基糠醛及其衍生物选择性加氢高效合成戊二醇催化剂的研究

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-04-17 DOI: 10.1039/d6cy00077k

Luyu Wang , Pengcheng Dai , Xin Li , Dandan Liu , Qian Gao , Zhaorui Zhang , Xin Gu , Liangjun Li , Mingbo Wu

The selective hydrogenation and ring-opening of furfural and its derivatives to pentanediols (PDOs) represent a potentially important route for promoting the sustainable production of bio-based fine chemicals. Due to the complex hydrogenation reaction network of furfural, achieving the catalytic hydrogenolysis of the C–O bond in the furan ring to target PDOs with high selectivity is a great challenge. Therefore, the rational design of heterogeneous catalysts is crucial. In this review, the catalyst designs for the hydrogenation of FF and its derivatives to PDOs are catalogued into three major products, 1,2-PDO, 1,5-PDO, and 1,4-PDO. Particular emphasis is placed on catalyst design strategies for the hydrogenation of FF and its derivatives to PDOs, including metal center modulation, support microenvironment engineering (including acidity/alkalinity, oxygen vacancies, and pore structure), and the synergistic effect of additives, to improve the catalytic activity, product selectivity, and catalyst stability. The reaction mechanisms are also discussed to provide insights for enhancing the selectivity and the design of multifunctional catalysts. Finally, future research is expected to focus on the precise design and rational regulation of catalytic systems, aiming to develop non-precious metal catalysts with higher efficiency, enhanced stability, and lower cost.

糠醛及其衍生物选择性加氢开环制戊二醇（PDOs）是促进生物基精细化学品可持续生产的重要途径。由于糠醛的加氢反应网络复杂，实现呋喃环上C-O键的催化氢解以高选择性的目标pdo是一个很大的挑战。因此，多相催化剂的合理设计至关重要。在本综述中，FF及其衍生物加氢成pdo的催化剂设计分为三种主要产品，1,2- pdo, 1,5- pdo和1,4- pdo。特别强调FF及其衍生物加氢成PDOs的催化剂设计策略，包括金属中心调制、支持微环境工程（包括酸/碱、氧空位和孔结构）以及添加剂的协同效应，以提高催化活性、产物选择性和催化剂稳定性。讨论了反应机理，为提高催化剂的选择性和设计多功能催化剂提供了参考。最后，未来的研究将集中在催化体系的精确设计和合理调控上，旨在开发效率更高、稳定性更强、成本更低的非贵金属催化剂。

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引用次数: 0

UV-laser-induced oxygen vacancy engineering of In(OH)3 for boosted CO2 photoreduction 紫外激光诱导In(OH)3氧空位工程促进CO2光还原

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-05-12 DOI: 10.1039/d6cy00159a

Zimu Zhang , Qiutong Han , Xiaotian Yang , Peiting Hao , Haoqiang Chi , Tingting Cheng , Yubin Zheng , Wentao Hou , Zhigang Zou , Yong Zhou

Efficient CO₂ photoreduction demands sufficient active sites and efficient separation of photogenerated charges. This work introduces ultraviolet laser-induced oxygen vacancy engineering to construct abundant oxygen defects in plate-like In(OH)₃, realizing excellent CO₂ photoreduction with a CO yield of 138.47 μmol g⁻¹ h⁻¹ and selectivity above 96%. Oxygen vacancies form mid-gap states to strengthen light harvesting, act as electron traps to promote carrier concentration and migration, and boost CO₂ adsorption and activation to facilitate *COOH formation. This strategy enriches active sites, optimizes charge separation, and regulates reaction pathways, and can be applied to large-area samples, showing broad application prospects.

有效的CO2光还原需要足够的活性位点和光生电荷的有效分离。本文引入紫外激光诱导氧空位工程，在类板状的in (OH)3中构建了丰富的氧缺陷，实现了良好的CO2光还原，CO产率达到138.47 μmol g−1 h−1，选择性达到96%以上。氧空位形成中隙态加强光捕获，作为电子陷阱促进载流子浓度和迁移，促进CO2吸附和活化，促进*COOH的形成。该策略丰富了活性位点，优化了电荷分离，调节了反应途径，可应用于大面积样品，具有广阔的应用前景。

引用次数: 0

Oxidative degradation of endocrine disruptor bisphenol-A on MnO2 nanosheets under ambient conditions 环境条件下二氧化锰纳米片上内分泌干扰物双酚a的氧化降解

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-04-16 DOI: 10.1039/d6cy00126b

Subhadeep Biswas , Vishnu Raj R , Sandip Saha , Ramkrishna Sahoo , Anjali Pal

Removal of bisphenol A (BPA) from water was studied using manganese dioxide nanoparticles prepared through co-precipitation using MnCl₂ and KMnO₄. The nanoparticles were observed to consist of nanosheets and are poorly crystalline as seen from the SEM and TEM images, XRD analysis, and SAED pattern. The pH_zpc of MnO₂ nanoparticles was observed to be 3.9. TGA studies of MnO₂ showed 13.5% weight loss. Specific capacitance was found to be 188 F g⁻¹ at a current of 1 A g⁻¹. The BPA–MnO₂ reaction was carried out under constant stirring under ambient conditions in an open-mouth glass tube. It was observed that about 80% of BPA was removed in 60 min for a MnO₂ dose of 1 g L⁻¹ and an initial BPA concentration of 50 mg L⁻¹. With an increase in the dosage of MnO₂, the removal efficiency increased, whereas it showed a decrease in the removal efficiency with an increase in the initial concentration of BPA. The rate of reaction was shown to be increasing with an increase in temperature and a decrease in pH. Kinetic studies indicated that it was a second-order reaction. Total organic carbon (TOC) removal was studied, and about 75% of TOC was removed in 60 minutes for the same dose and initial concentration. Metal ions such as Ca²⁺ and Fe³⁺ decreased the final removal efficiency. A slight leaching of Mn²⁺ ions was observed during the course of the reaction, which confirmed the oxidative degradation of BPA. The reaction was carried out in a nitrogen environment. It was observed that oxygen had a minor role in the BPA degradation. Transformation products were identified by mass spectrometric studies.

研究了二氧化锰纳米颗粒（MnCl2和KMnO4共沉淀法）对水中双酚A的去除效果。从SEM、TEM、XRD和SAED图上可以看出，纳米颗粒由纳米片组成，结晶度较差。MnO2纳米颗粒的pHzpc为3.9。MnO2的TGA研究显示体重减轻13.5%。在电流为1ag−1时，比电容为188fg−1。在常压条件下，在开口玻璃管中不断搅拌进行BPA-MnO2反应。在MnO2浓度为1 g L−1，初始BPA浓度为50 mg L−1的条件下，60 min内BPA去除率约为80%。随着MnO2投加量的增加，去除率提高，而随着BPA初始浓度的增加，去除率降低。反应速率随温度的升高和ph的降低而增大，动力学研究表明该反应为二级反应。对总有机碳（TOC）的去除率进行了研究，在相同的初始浓度和剂量下，60分钟内TOC去除率约为75%。Ca2+和Fe3+等金属离子降低了最终的去除效率。在反应过程中观察到Mn2+离子的轻微浸出，证实了BPA的氧化降解。该反应在含氮环境中进行。结果表明，氧对双酚a的降解作用较小。转化产物经质谱分析鉴定。

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引用次数: 0

Engineering spatial and electrostatic confinement in zeolites for enhanced low-temperature NO oxidation 沸石中强化低温NO氧化的工程空间和静电约束

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-04-28 DOI: 10.1039/d6cy00268d

Guang-Wei Ma , Qi Chen , Sai Zhang , Yuan-Hang Qin , Zhen Chen , Li Yang , Cun-Wen Wang

Low-temperature catalytic oxidation of nitric oxide (NO) has drawn significant attention, underscoring the need for catalysts with enhanced activity in the low-temperature regime. Zeolites possess intrinsic advantages for NO oxidation, as their confined microporous frameworks can stabilize the transition state (TS) through enthalpic interactions while mitigating entropy loss, thereby enabling efficient catalysis at reduced temperatures. To achieve stronger confinement of the NO oxidation TS and consequently improve catalytic performance, a three-step zeolite optimization strategy was developed to simultaneously regulate spatial and electrostatic environments within the framework. First, a zeolite with appropriate void spaces was selected; second, its Si/Al ratio (SAR) was adjusted to fine-tune the framework properties; and third, ion exchange was conducted to further modulate spatial and electrostatic effects. The results indicate that both pore size and extra-framework cations play critical roles in governing the catalytic activity of zeolites for NO oxidation. Among the synthesized materials, potassium-exchanged SSZ-13 with an SAR of 8 (K-SSZ-13-8) exhibited the highest low-temperature NO oxidation activity, achieving 87.2% of NO conversion at 25 °C, along with relatively good tolerance to sulfur dioxide. This study provides a rational design strategy for developing high-performance zeolite catalysts for low-temperature NO oxidation.

一氧化氮（NO）的低温催化氧化引起了极大的关注，强调了在低温条件下具有增强活性的催化剂的需求。沸石具有氧化NO的内在优势，因为其受限的微孔框架可以通过焓相互作用稳定过渡态（TS），同时减轻熵损失，从而在低温下实现高效催化。为了实现对NO氧化TS的更强约束，从而提高催化性能，研究人员开发了一种三步沸石优化策略，以同时调节框架内的空间和静电环境。首先，选择具有适当空隙的沸石；其次，通过调整硅铝比（SAR）来微调骨架性能；第三，离子交换进一步调节空间和静电效应。结果表明，孔径和框架外阳离子对沸石氧化NO的催化活性起关键作用。在合成的材料中，SAR为8的换钾SSZ-13 （K-SSZ-13-8）的低温NO氧化活性最高，在25℃时NO转化率达到87.2%，并且具有较好的耐二氧化硫能力。本研究为开发高性能低温NO氧化沸石催化剂提供了合理的设计策略。

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引用次数: 0

Electrochemical reconstruction leading to a borate-linked [Co(Fe)]8B2O16H2 crystalline phase for the efficient and stable OER 电化学重建导致硼酸连接的[Co(Fe)]8B2O16H2晶相高效稳定的OER

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-04-30 DOI: 10.1039/d6cy00100a

Xing-Hui Zhang , Yi-Fan Hu , Zhi-Pan Liu

Recent developments relating to oxygen evolution reaction (OER) catalysts have shifted to multiple-element or even high-entropy materials for achieving high activity and high stability, but clarification of the synergistic mechanism between elements has been challenging. Here, by utilizing state-of-the-art machine-learning-based global structure exploration and electrochemical experiments, we show that in iron, boron and cobalt ternary oxide catalysts, Co_xFe_yB_z with x : y : z = 4 : 1 : 1, the initially amorphous material reconstructs into a crystalline phase with the formula [Co(Fe)]₈B₂O₁₆H₂, featuring borate (BO₃)-linked CoO₂ layers exposing Fe cation sites. This borate-linked structure delivers rational performance metrics and, more importantly, exhibits exceptional and multifaceted stability: it retains 97% of its initial stability after 200 h of chronoamperometric testing, shows almost no voltage change after multi-current step testing, and maintains a stable potential throughout 200 h of intermittent testing (12 h start–shutdown cycles at 10 mA cm⁻²) in 1 M KOH electrolyte. While boron acts as the structural skeleton dopant, iron not only stabilizes the Co(Fe)O₂ layer surfaces but also enhances the OER activity by markedly stabilizing the key terminal O* and OOH* intermediates by ∼0.50 eV, giving rise to a characteristic Raman peak at 940 cm⁻¹.

近年来，为了获得高活性和高稳定性，出氧反应（OER）催化剂已转向多元素甚至高熵材料，但澄清元素之间的协同作用机制一直具有挑战性。在这里，通过利用最先进的基于机器学习的全局结构探索和电化学实验，我们发现，在铁、硼和钴三元氧化物催化剂CoxFeyBz （x: y: z = 4:1:1）中，最初的无定形材料重构为公式为[Co(Fe)]8B2O16H2的结晶相，其特征是硼酸盐（BO3）连接的CoO2层暴露出Fe阳离子位点。这种硼酸盐连接结构提供了合理的性能指标，更重要的是，表现出卓越的多方面稳定性：在200小时的计时安培测试后，它保持了97%的初始稳定性，在多电流阶跃测试后几乎没有电压变化，并在1 M KOH电解质中进行200小时的间歇测试（10 mA cm - 2下12小时的启停周期）保持稳定的电位。当硼作为结构骨架掺杂时，铁不仅稳定了Co(Fe)O2层表面，而且通过将关键末端O*和OOH*中间体显著稳定约0.50 eV，提高了OER活性，在940 cm−1处产生特征拉曼峰。

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引用次数: 0

Catalytic studies of Pt supported on Co/CeO2 nanorods for H2 production in dry reforming of methane Co/CeO2纳米棒负载Pt催化甲烷干重整制氢的研究

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-04-24 DOI: 10.1039/d5cy01416f

J. Reyna-Alvarado , Jorge Trimmer-Duarte , Oscar Recalde-Benitez , Leopoldo Molina-Luna , Albina Gutiérrez-Martínez , Gilberto Mondragón-Galicia , Manuel Ramos , Raúl Pérez-Hernández

An integrated experimental–theoretical study was performed on 15Co/CeO₂ nanorod catalysts with varying Pt loadings (0.1–0.5 wt%) for dry reforming of methane (DRM) to syngas. CeO₂ nanorods were synthesized hydrothermally and sequentially impregnated with Co and Pt. The catalysts were characterized by XRD, TPR, TPO, CO₂- and NH₃-TPD, and TEM/STEM-EDX, while DFT calculations were conducted to evaluate the proposed reaction mechanism and transition states. TEM revealed isolated Pt and Co nanoparticles anchored to CeO₂ surfaces. The monometallic Co/CeO₂-NR catalyst exhibited pronounced deactivation and significant sintering, whereas Pt-promoted catalysts showed enhanced stability despite increased graphitic carbon deposition. Post-reaction SEM and TEM indicated partial detachment of the active phase associated with carbon nanotube growth which contributes to catalyst deactivation. Energy transition state profiles by Halgren–Lipscomb showed no significant decrease in activation energy with increasing Pt content; however, catalytic tests demonstrated higher reactant conversions, suggesting that Pt enhances DRM performance through mechanisms beyond simple energy barrier reduction.

对不同Pt负载（0.1-0.5 wt%）的15Co/CeO2纳米棒催化剂用于甲烷（DRM）干重整制合成气进行了综合实验-理论研究。采用水热法合成了CeO2纳米棒，并依次浸渍Co和Pt。采用XRD、TPR、TPO、CO2-和NH3-TPD、TEM/STEM-EDX对催化剂进行了表征，并通过DFT计算对反应机理和过渡态进行了评价。透射电镜显示分离的Pt和Co纳米颗粒锚定在CeO2表面。单金属Co/CeO2-NR催化剂表现出明显的失活和明显的烧结，而pt促进的催化剂表现出更高的稳定性，尽管石墨碳沉积增加。反应后的扫描电镜和透射电镜显示，碳纳米管生长过程中活性相部分脱落，导致催化剂失活。Halgren-Lipscomb能量过渡态谱显示，随着Pt含量的增加，活化能没有显著降低；然而，催化测试显示了更高的反应物转化率，这表明Pt通过简单的能量势垒还原之外的机制提高了DRM性能。

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引用次数: 0

Preparation of CuCo/NH2-MIL-101(Fe) nanocomposite for photocatalytic synthesis of 2,3-dihydroquinazolin-4(1H)-ones and 1-amidoalkyl-2-naphthols CuCo/NH2-MIL-101（Fe）纳米复合材料光催化合成2,3-二氢喹唑啉-4(1H)-酮和1-氨基烷基-2-萘酚的制备

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-05-14 DOI: 10.1039/d5cy01583a

Neda Cheraghi , Mohammad Jafarzadeh

Bimetallic CuCo nanoparticles were grown on iron-based NH₂-MIL-101 metal–organic frameworks, and their photoactivity was evaluated for photocatalytic organic synthesis. The CuCo/NH₂-MIL-101 composite exhibited a narrower bandgap (E_g = 1.3 eV), slower photogenerated charge recombination, enhanced charge separation, and faster charge transport compared to pristine NH₂-MIL-101 (E_g = 1.48 eV). As a photocatalyst, CuCo/NH₂-MIL-101 enabled light-driven synthesis of 2,3-dihydroquinazolin-4(1H)-one derivatives with 83–93% yields in 2–2.5 h under visible light irradiation (200 W LED lamp). It also efficiently catalyzed the synthesis of 1-amidoalkyl-2-naphthols, achieving 78–95% yields in 70–105 min (200 W LED lamp). The synergistic effect between Cu and Co, combined with the intrinsic photoactivity of NH₂-MIL-101, significantly enhanced the composite's photocatalytic performance. Moreover, the photocatalyst demonstrated excellent functional and structural stability over five recycling runs.

在铁基NH2-MIL-101金属有机骨架上生长了双金属cuo纳米颗粒，并对其光催化有机合成进行了光活性评价。与原始NH2-MIL-101 （Eg = 1.48 eV）相比，CuCo/NH2-MIL-101复合材料具有更窄的带隙（Eg = 1.3 eV）、更慢的光生电荷重组、更强的电荷分离和更快的电荷传输。CuCo/NH2-MIL-101作为光催化剂，在200 W LED灯的可见光照射下，在2- 2.5 h内催化合成2,3-二氢喹唑啉-4(1H)- 1衍生物，产率为83-93%。它还能高效催化1-氨基烷基-2-萘酚的合成，在70-105 min （200 W LED灯）下，收率达到78-95%。Cu和Co之间的协同作用，结合NH2-MIL-101的固有光活性，显著增强了复合材料的光催化性能。此外，光催化剂在五次循环运行中表现出优异的功能和结构稳定性。

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引用次数: 0

Photothermal flash light doping of strontium titanate photocatalyst nanoparticles 光热闪光掺杂钛酸锶光催化剂纳米颗粒

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-05-07 DOI: 10.1039/d5cy01501d

Melanie Johanning , Wanderson O. Silva , Anselm Dreher , Paul Kant , Mara Blöchlinger , Arthur E. Bouchez , Coral Felipe Gracia , Hannah Johnson , Roland Dittmeyer , Mathieu Soutrenon , Kevin Sivula

Rhodium and lanthanum co-doped strontium titanate (Rh,La:SrTiO₃) is a promising material for green hydrogen (H₂) production via heterogeneous photocatalytic (PC) water splitting. State-of-the-art Rh,La:SrTiO₃ nanoparticle photocatalysts mitigate charge recombination using an undoped core/doped shell structure. However, the typically-employed synthesis methods use high temperatures >1000 °C in a slow dopant diffusion process, which induces inhomogeneities, causes nanoparticle sintering, and limits material performance. In this work, we demonstrate a rapid flash light annealing (FLA) technique that affords suitable nanoparticle doping in only 7.5 seconds. FLA samples show a PC performance three times greater than conventional thermal doping, which we attribute to mitigated particle sintering and dopants incorporated closer to the surface. Moreover, the H₂ evolution rate under full spectrum simulated solar illumination increased by 50% compared to the undoped precursor nanoparticles. Finally, varying the flash parameters shows the tunability of the FLA process. The developed method paves the way for extending rapid doping by FLA to other powdered materials without the need for ion implantation.

铑镧共掺杂钛酸锶（Rh,La:SrTiO3）是一种很有前途的非均相光催化（PC）水裂解绿色制氢材料。最先进的Rh，La:SrTiO3纳米颗粒光催化剂使用未掺杂的核/掺杂的壳结构减轻电荷重组。然而，通常采用的合成方法在掺杂剂缓慢扩散过程中使用高温（1000℃），这会导致不均匀性，导致纳米颗粒烧结，并限制材料性能。在这项工作中，我们展示了一种快速闪光退火（FLA）技术，该技术仅在7.5秒内提供合适的纳米颗粒掺杂。FLA样品的PC性能是传统热掺杂的三倍，我们将其归因于减轻颗粒烧结和更靠近表面的掺杂剂。此外，在全光谱模拟太阳光照下，H2的析出速率比未掺杂的纳米前驱体提高了50%。最后，改变闪光参数显示了FLA过程的可调性。该方法为在不需要离子注入的情况下将FLA快速掺杂到其他粉末材料中铺平了道路。

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引用次数: 0

Synergistic photocatalytic production of H2O2 and imines via oxygen-enriched acetonitrile medium and benzylamine oxidation 富氧乙腈介质和苄胺氧化协同光催化生产H2O2和亚胺

IF 4.2 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology

Pub Date : 2026-06-08 Epub Date: 2026-04-23 DOI: 10.1039/d6cy00178e

Xin Xu , Yuming Dong , Yingxin Guo , Xinxin Jiang , Lizi Liu , Tingyu Yang , Xinyu Sun , Pengken Li , Hui Zhao , Yongfa Zhu , Junshan Li

Photocatalytic technology has emerged as a sustainable and efficient strategy for chemical synthesis, yet its application in H₂O₂ production is limited by low dissolved oxygen availability and inefficient charge carrier utilization. To overcome these limitations, we developed an innovative photocatalytic system that uses acetonitrile as the solvent. Due to its markedly higher oxygen solubility compared to water, this system significantly improves oxygen mass transfer and overall reaction kinetics. Furthermore, we introduced benzylamine oxidation as an alternative to the conventional water oxidation reaction. Benefiting from its favorable oxidation potential, the oxidation of benzylamine not only requires lower energy input, but also couples synergistically with H₂O₂ generation, forming a bifunctional catalytic system that significantly enhances the efficiency of H₂O₂ synthesis. The system achieves a high H₂O₂ production rate of 12.03 mmol g⁻¹ h⁻¹ and a concentration of 28.9 mmol L⁻¹, significantly outperforming conventional aqueous-phase systems. Subsequent distillation and extraction processes concentrated the aqueous H₂O₂ solution to 413.43 mM (>1 wt%), approaching the concentration of medical-grade H₂O₂. Mechanistic investigations confirm that the reaction follows a two-electron oxygen reduction pathway. This work not only presents a novel and sustainable route for H₂O₂ production, but also demonstrates potential for photocatalytic synthesis of other high-value chemicals.

光催化技术已成为一种可持续和高效的化学合成策略，但其在H2O2生产中的应用受到溶解氧利用率低和载流子利用率低的限制。为了克服这些限制，我们开发了一种创新的光催化系统，使用乙腈作为溶剂。由于其氧溶解度明显高于水，该体系显著改善了氧传质和整体反应动力学。此外，我们还介绍了一种替代传统水氧化反应的苯胺氧化反应。得益于其良好的氧化电位，苯胺的氧化不仅需要较低的能量输入，而且与H2O2的生成协同耦合，形成双功能催化体系，显著提高H2O2的合成效率。该体系的H2O2产率为12.03 mmol g−1 h−1，浓度为28.9 mmol L−1，明显优于传统的水相体系。随后的蒸馏和萃取过程将H2O2水溶液浓缩到413.43 mM (>1 wt%)，接近医用级H2O2的浓度。机理研究证实该反应遵循双电子氧还原途径。这项工作不仅为H2O2的生产提供了一种新的、可持续的途径，而且还展示了光催化合成其他高价值化学品的潜力。

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引用次数: 0