Materials Today Catalysis最新文献_第3页

Cover 封面

Materials Today Catalysis

Pub Date : 2025-06-01 DOI: 10.1016/S2949-754X(25)00020-1

引用次数: 0

Microelectrochemical investigation of electrocatalytic hydrogen evolution reaction 电催化析氢反应的微电化学研究

Materials Today Catalysis

Pub Date : 2025-06-01 DOI: 10.1016/j.mtcata.2025.100106

Kai Bao , Cong Ma , Lingzhi Wang , Ruijie Li , Wenbin Wang , Zongxiao Wu , Wei Zhai , Jingkun Wu , Chengxuan Ke , Zhixiang Tao , Zhuangzhuang Yin , Junlei Qi , Qiyuan He

Electrocatalytic hydrogen evolution reaction (HER), as a green and sustainable method of hydrogen production, has attracted wide attention in recent years. Designing electrocatalysts with high efficiency, low-cost and stability for HER is becoming increasingly promising and feasible. The emerging microelectrochemical investigation has proven to be a highly effective tool in uncovering complex catalytic mechanism, particularly in HER of single-entity nanocatalysts. Among the various microelectrochemical methods, ultramicroelectrode (UME) and on-chip electrochemical microcell (OCEM) are mostly widely regarded. Both techniques have been extensively employed to analysis the HER process of single-entity nanomaterials, giving unique perspectives inaccessible to conventional electrochemical methods. This review outlines the principles and compares the similarities and differences among UME, OCEM and conventional electrochemical methods. The applications of UME and OCEM investigation of specific nanocatalyts, especially 2D materials, are comprehensively reviewed. Finally, challenges and outlook of microelectrochemical methods in electrocatalysis and beyond are discussed.

电催化析氢反应（HER）作为一种绿色可持续的制氢方法，近年来受到了广泛的关注。设计高效、低成本、稳定的HER电催化剂正变得越来越有前景和可行性。新兴的微电化学研究已被证明是揭示复杂催化机理的有效工具，特别是在单实体纳米催化剂的HER中。在各种微电化学方法中，超微电极（UME）和片上电化学微电池（OCEM）最受关注。这两种技术都被广泛用于分析单实体纳米材料的HER过程，提供了传统电化学方法无法获得的独特视角。本文概述了UME、OCEM和常规电化学方法的原理，并比较了它们的异同。综述了UME和OCEM在特定纳米催化剂，特别是二维材料研究中的应用。最后，讨论了微电化学方法在电催化及其他领域所面临的挑战和前景。

{"title":"Microelectrochemical investigation of electrocatalytic hydrogen evolution reaction","authors":"Kai Bao , Cong Ma , Lingzhi Wang , Ruijie Li , Wenbin Wang , Zongxiao Wu , Wei Zhai , Jingkun Wu , Chengxuan Ke , Zhixiang Tao , Zhuangzhuang Yin , Junlei Qi , Qiyuan He","doi":"10.1016/j.mtcata.2025.100106","DOIUrl":"10.1016/j.mtcata.2025.100106","url":null,"abstract":"<div><div>Electrocatalytic hydrogen evolution reaction (HER), as a green and sustainable method of hydrogen production, has attracted wide attention in recent years. Designing electrocatalysts with high efficiency, low-cost and stability for HER is becoming increasingly promising and feasible. The emerging microelectrochemical investigation has proven to be a highly effective tool in uncovering complex catalytic mechanism, particularly in HER of single-entity nanocatalysts. Among the various microelectrochemical methods, ultramicroelectrode (UME) and on-chip electrochemical microcell (OCEM) are mostly widely regarded. Both techniques have been extensively employed to analysis the HER process of single-entity nanomaterials, giving unique perspectives inaccessible to conventional electrochemical methods. This review outlines the principles and compares the similarities and differences among UME, OCEM and conventional electrochemical methods. The applications of UME and OCEM investigation of specific nanocatalyts, especially 2D materials, are comprehensively reviewed. Finally, challenges and outlook of microelectrochemical methods in electrocatalysis and beyond are discussed.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100106"},"PeriodicalIF":0.0,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144253684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Superior reversible hydrogen storage in eutectic LiBH4–KBH4 system via Ni–based catalysts synergized with graphene 镍基催化剂与石墨烯协同作用在LiBH4-KBH4共晶体系中具有优异的可逆储氢性能

Materials Today Catalysis

Pub Date : 2025-05-27 DOI: 10.1016/j.mtcata.2025.100105

Shanqing Qu , Yaxiong Yang , Mingxia Gao , Zhenglong Li , Wenping Sun , Chu Liang , Xin Zhang , Xiaoyu Zhang , Lingchao Zhang , Ruizi Wang , Hongge Pan

Light metal borohydrides are promising candidates for solid–state hydrogen storage due to their high hydrogen storage capacities; however, the reversibility and kinetics of de/hydrogenation still require significant improvement. The present work focuses on the improvement of the hydrogen storage properties of the eutectic borohydride system of LiBH₄–KBH₄ (Li/KBH₄). A layered composite of graphene supported with ultrafine Ni₃B nanoparticles (Ni₃B/G) is designed and synthesized, which acts as catalyst and confinement carrier for Li/KBH₄. Assisted with a heating of the mixture of Li/KBH₄ and Ni₃B/G to 110 °C in the molten state of Li/KBH₄, an interlayer structure of graphene dispersed with Ni₃B nanoparticles and sheet–like Li/KBH₄ is constructed. The graphene effectively disperses Ni₃B nanoparticles and confines the Li/KBH₄ in its interlayers. The confinement of Li/KBH₄ and the catalysis of Ni₃B nanoparticles, assisted with the high thermal conductivity of graphene, contribute synergistically the hydrogen storage of Li/KBH₄. The main dehydrogenation peak temperature of the system is lowered to 278 °C. The system can release 8.5 wt% H₂ within 30 min at 350 °C. The capacity retention achieves 81.2 % after 50 cycles. DFT theoretical analysis shows that there is strong charge transfer interaction between Ni₃B and LiBH₄/KBH₄, which destabilizes the [BH₄]^– structure and promotes the dehydrogenation. This work provides a new approach for the design of new structural LiBH₄–based eutectic system with high capacity, low dehydrogenation temperature, high reversibility and long cycling life.

轻金属硼氢化物因其高储氢能力而成为固态储氢的有希望的候选者；然而，脱氢化反应的可逆性和动力学仍有待改进。本文主要研究了LiBH4-KBH4 （Li/KBH4）共晶硼氢化物体系储氢性能的改进。设计并合成了一种层状石墨烯-超细Ni3B纳米颗粒复合材料（Ni3B/G），作为Li/KBH4的催化剂和约束载体。在Li/KBH4熔融状态下，将Li/KBH4和Ni3B/G的混合物加热至110℃，构建了分散有Ni3B纳米粒子和片状Li/KBH4的石墨烯层间结构。石墨烯有效地分散了Ni3B纳米颗粒，并将Li/KBH4限制在其中间层中。Li/KBH4的约束和Ni3B纳米颗粒的催化作用，以及石墨烯的高导热性，协同促进了Li/KBH4的储氢。系统主脱氢峰温度降至278℃。该系统在350℃下可在30 min内释放8.5 wt% H2。循环50次后，容量保持率达到81.2 %。DFT理论分析表明，Ni3B与LiBH4/KBH4之间存在较强的电荷转移相互作用，使[BH4] -结构不稳定，促进了脱氢反应。本工作为设计高容量、低脱氢温度、高可逆性和长循环寿命的新型结构libh4共晶体系提供了新途径。

{"title":"Superior reversible hydrogen storage in eutectic LiBH4–KBH4 system via Ni–based catalysts synergized with graphene","authors":"Shanqing Qu , Yaxiong Yang , Mingxia Gao , Zhenglong Li , Wenping Sun , Chu Liang , Xin Zhang , Xiaoyu Zhang , Lingchao Zhang , Ruizi Wang , Hongge Pan","doi":"10.1016/j.mtcata.2025.100105","DOIUrl":"10.1016/j.mtcata.2025.100105","url":null,"abstract":"<div><div>Light metal borohydrides are promising candidates for solid–state hydrogen storage due to their high hydrogen storage capacities; however, the reversibility and kinetics of de/hydrogenation still require significant improvement. The present work focuses on the improvement of the hydrogen storage properties of the eutectic borohydride system of LiBH<sub>4</sub>–KBH<sub>4</sub> (Li/KBH<sub>4</sub>). A layered composite of graphene supported with ultrafine Ni<sub>3</sub>B nanoparticles (Ni<sub>3</sub>B/G) is designed and synthesized, which acts as catalyst and confinement carrier for Li/KBH<sub>4</sub>. Assisted with a heating of the mixture of Li/KBH<sub>4</sub> and Ni<sub>3</sub>B/G to 110 °C in the molten state of Li/KBH<sub>4</sub>, an interlayer structure of graphene dispersed with Ni<sub>3</sub>B nanoparticles and sheet–like Li/KBH<sub>4</sub> is constructed. The graphene effectively disperses Ni<sub>3</sub>B nanoparticles and confines the Li/KBH<sub>4</sub> in its interlayers. The confinement of Li/KBH<sub>4</sub> and the catalysis of Ni<sub>3</sub>B nanoparticles, assisted with the high thermal conductivity of graphene, contribute synergistically the hydrogen storage of Li/KBH<sub>4</sub>. The main dehydrogenation peak temperature of the system is lowered to 278 °C. The system can release 8.5 wt% H<sub>2</sub> within 30 min at 350 °C. The capacity retention achieves 81.2 % after 50 cycles. DFT theoretical analysis shows that there is strong charge transfer interaction between Ni<sub>3</sub>B and LiBH<sub>4</sub>/KBH<sub>4</sub>, which destabilizes the [BH<sub>4</sub>]<sup>–</sup> structure and promotes the dehydrogenation. This work provides a new approach for the design of new structural LiBH<sub>4</sub>–based eutectic system with high capacity, low dehydrogenation temperature, high reversibility and long cycling life.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100105"},"PeriodicalIF":0.0,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144169432","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Photocatalytic transformation of organic pollutants and remediation strategies of carbon emissions and nitrogen fixation in inland water 内陆水体有机污染物的光催化转化及碳排放固氮修复策略

Materials Today Catalysis

Pub Date : 2025-05-09 DOI: 10.1016/j.mtcata.2025.100103

Masiha Rahman, Saman Shaheen, Tokeer Ahmad

Photocatalysis is an environmentally friendly approach and a propitious avenue for addressing water contamination including toxic chemicals, radioactive materials, and nitrate fertilizer. In the past few years, urbanization and industrialization have affected the water quality, causing various environmental hazards. Inland water ecosystems such as lakes, rivers and wetland not only play a vital role in maintaining biodiversity but also provide important sources of GHGs emissions. Despite their significance, the emission from inland water is poorly quantified. This review systematically reveals the sources of carbon and nitrogen emissions, the efficiency and mechanisms of various photocatalysts in degrading a range of organic pollutants, highlighting their potential to reduce environmental toxins significantly. The state-of-the-art and innovative remediation strategies targeting carbon emissions and N₂ fixation have been thoroughly discussed. By consolidating photocatalytic processes with carbon sequestration and N₂ fixation, the review develops a holistic approach to alleviating water quality and mitigating climate change impacts. Finally, the findings concluded with the role of advanced photocatalytic materials and proffering perspectives in promoting sustainable environmental management and ecological health in inland aquatic systems.

光催化是一种环境友好的方法，是解决包括有毒化学物质、放射性物质和硝酸盐肥料在内的水污染的有利途径。在过去的几年里，城市化和工业化已经影响了水质，造成了各种环境危害。湖泊、河流和湿地等内陆水域生态系统不仅在维持生物多样性方面发挥着至关重要的作用，也是温室气体排放的重要来源。尽管它们意义重大，但内陆水域的排放却难以量化。本文系统地揭示了碳和氮排放的来源，各种光催化剂降解一系列有机污染物的效率和机制，强调了它们在显著减少环境毒素方面的潜力。深入讨论了针对碳排放和氮固定的最新和创新的修复策略。通过将光催化过程与固碳和固氮结合起来，本文提出了一种改善水质和减轻气候变化影响的整体方法。最后，总结了先进光催化材料在促进内陆水生系统可持续环境管理和生态健康方面的作用，并提出了展望。

{"title":"Photocatalytic transformation of organic pollutants and remediation strategies of carbon emissions and nitrogen fixation in inland water","authors":"Masiha Rahman, Saman Shaheen, Tokeer Ahmad","doi":"10.1016/j.mtcata.2025.100103","DOIUrl":"10.1016/j.mtcata.2025.100103","url":null,"abstract":"<div><div>Photocatalysis is an environmentally friendly approach and a propitious avenue for addressing water contamination including toxic chemicals, radioactive materials, and nitrate fertilizer. In the past few years, urbanization and industrialization have affected the water quality, causing various environmental hazards. Inland water ecosystems such as lakes, rivers and wetland not only play a vital role in maintaining biodiversity but also provide important sources of GHGs emissions. Despite their significance, the emission from inland water is poorly quantified. This review systematically reveals the sources of carbon and nitrogen emissions, the efficiency and mechanisms of various photocatalysts in degrading a range of organic pollutants, highlighting their potential to reduce environmental toxins significantly. The state-of-the-art and innovative remediation strategies targeting carbon emissions and N<sub>2</sub> fixation have been thoroughly discussed. By consolidating photocatalytic processes with carbon sequestration and N<sub>2</sub> fixation, the review develops a holistic approach to alleviating water quality and mitigating climate change impacts. Finally, the findings concluded with the role of advanced photocatalytic materials and proffering perspectives in promoting sustainable environmental management and ecological health in inland aquatic systems.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100103"},"PeriodicalIF":0.0,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143929593","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

VN/Copper foam self-supporting catalyst for efficient electrocatalytic hydrogen peroxide generation 用于高效电催化过氧化氢生成的VN/铜泡沫自支撑催化剂

Materials Today Catalysis

Pub Date : 2025-05-09 DOI: 10.1016/j.mtcata.2025.100102

Jiahao Liu , Zhaorui Zhang , Chenshuai Han, Minghui Yang

Hydrogen peroxide (H₂O₂) is a crucial chemical, while its conventional production methods are energy-intensive and environmentally damaging. Electrocatalytic synthesis of H₂O₂ through 2e^- oxygen reduction reaction (ORR) presents a sustainable alternative. Here, we introduce a novel VN/Copper foam (VN/CF) self-supporting catalyst, achieving an H₂O₂ production yield rate of 169.7 mg·h⁻¹·cm⁻² with a Faradaic efficiency (FE) of 89.1 %. The self-supporting VN/CF demonstrates remarkable durability, sustaining stable operation at a current density of 300 mA cm⁻² over 110 h. Notably, the capital cost of 70 wt% H₂O₂ is remarkably low at just $0.25/kg. This work highlights the potential of self-supported metal nitrides as stable and efficient 2e^- ORR catalysts.

过氧化氢（H2O2）是一种至关重要的化学物质，而其传统的生产方法是能源密集型的，并且对环境有害。通过2e-氧还原反应（ORR）电催化合成H2O2是一种可持续的替代方法。本文介绍了一种新型的VN/Copper foam （VN/CF）自支撑催化剂，其H2O2产率为169.7 mg·h−1·cm−2，法拉第效率（FE）为89.1% %。自支撑型VN/CF具有出色的耐久性，在电流密度为300 mA cm−2超过110 h时保持稳定运行。值得注意的是，70 wt% H2O2的投资成本非常低，仅为0.25美元/公斤。这项工作突出了自支撑金属氮化物作为稳定和高效的2e- ORR催化剂的潜力。

引用次数: 0

Advances in understanding and manipulating electrode wettability for electrocatalytic performance enhancement 提高电催化性能的电极润湿性研究进展

Materials Today Catalysis

Pub Date : 2025-05-07 DOI: 10.1016/j.mtcata.2025.100101

Hailing Zhao , Kaijie Ma , Shiqin Gao , Bolun Wang , Yang Wang

In the realm of heterogeneous catalysis, the wettability of the catalyst significantly impacts the interaction between the catalyst surface and reactants or products, thereby playing a pivotal role in determining catalytic performance. Electrocatalytic reactions predominantly occur at multiphase interfaces. As a result, gas-liquid-solid interface mass transfer is of utmost importance during the reaction process. In the electrocatalysis process, for steps including molecular adsorption, desorption, and surface transfer, the modulation of electrode wettability directly influences the behavior of gas bubbles beneath the solution. This affects the gas-liquid-solid interface mass transfer process during electrocatalysis. Consequently, a comprehensive understanding of the principles governing this interfacial interaction is crucial for fundamentally enhancing the efficiency of electrocatalytic reactions. This review summarizes the basic theory of wettability and its relationship with electrocatalytic reactions. It also accentuates some recent advancements in the impact of electrode wettability in heterogeneous electrocatalytic reactions. Finally, the review offers a perspective on the challenges associated with wettability regulation in influencing the electrocatalytic reaction process.

在多相催化领域，催化剂的润湿性显著影响催化剂表面与反应物或产物的相互作用，从而在决定催化性能方面起着举足轻重的作用。电催化反应主要发生在多相界面。因此，气-液-固界面传质在反应过程中起着至关重要的作用。在电催化过程中，对于包括分子吸附、解吸和表面转移在内的步骤，电极润湿性的调节直接影响溶液下气泡的行为。这影响了电催化过程中气-液-固界面传质过程。因此，全面了解控制这种界面相互作用的原理对于从根本上提高电催化反应的效率至关重要。本文综述了润湿性的基本理论及其与电催化反应的关系。它还强调了在非均相电催化反应中电极润湿性影响方面的一些最新进展。最后，本文对影响电催化反应过程的润湿性调控所面临的挑战进行了展望。

{"title":"Advances in understanding and manipulating electrode wettability for electrocatalytic performance enhancement","authors":"Hailing Zhao , Kaijie Ma , Shiqin Gao , Bolun Wang , Yang Wang","doi":"10.1016/j.mtcata.2025.100101","DOIUrl":"10.1016/j.mtcata.2025.100101","url":null,"abstract":"<div><div>In the realm of heterogeneous catalysis, the wettability of the catalyst significantly impacts the interaction between the catalyst surface and reactants or products, thereby playing a pivotal role in determining catalytic performance. Electrocatalytic reactions predominantly occur at multiphase interfaces. As a result, gas-liquid-solid interface mass transfer is of utmost importance during the reaction process. In the electrocatalysis process, for steps including molecular adsorption, desorption, and surface transfer, the modulation of electrode wettability directly influences the behavior of gas bubbles beneath the solution. This affects the gas-liquid-solid interface mass transfer process during electrocatalysis. Consequently, a comprehensive understanding of the principles governing this interfacial interaction is crucial for fundamentally enhancing the efficiency of electrocatalytic reactions. This review summarizes the basic theory of wettability and its relationship with electrocatalytic reactions. It also accentuates some recent advancements in the impact of electrode wettability in heterogeneous electrocatalytic reactions. Finally, the review offers a perspective on the challenges associated with wettability regulation in influencing the electrocatalytic reaction process.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100101"},"PeriodicalIF":0.0,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143929592","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles 研究镍纳米颗粒在苯甲醛还原胺化反应中的尺寸依赖性选择性

Materials Today Catalysis

Pub Date : 2025-04-29 DOI: 10.1016/j.mtcata.2025.100100

Yunong Li , Ching Kit Tommy Wun , Tianxiang Chen , Tsz Woon Benedict Lo

Selectivity control is a fundamental focus in catalysis chemistry, as it directly reflects the efficiency and efficacy of catalytic processes. While catalysis often involves intricate and cascade reaction steps using nanoparticle (NP) catalysts, the mechanism behind the size effect of nanoparticles on product selectivity has not been fully explored. We herein prepared a series of Ni-containing zeolitic catalysts in which the Ni NPs are uniformly supported on the mesopores and outer surfaces of H-ZSM-5 zeolites. The dynamic formation of Ni NPs from highly dispersed Ni precursors was monitored using transmission electron microscopy, in-situ X-ray pair distribution function, and in-situ X-ray absorption fine structure analysis. The metal nanoparticle size was carefully controlled between 3.72(5) nm and 11.91(7) by controlling the reduction temperature. We evaluated the catalytic performance of Ni NPs using the reductive amination of benzaldehyde in batch reactors at low temperatures. This reaction inherently favors the formation of a series of products, suffering highly from selectivity issues. Our results revealed a size-dependent behavior in reaction efficiency, with the catalyst achieving the highest catalytic activity (93 % selectivity in primary amine) at a particle size of 5.62(3) nm. This optimal performance is attributed to a balanced interplay between hydrogenation and amination capabilities. These findings highlight the intricate relationship between nanoparticle size and catalytic performance, emphasizing the necessity for precise optimization in catalyst design to enhance selectivity and sustainability in industrial applications.

选择性控制是催化化学中的一个基本问题，因为它直接反映了催化过程的效率和效果。虽然使用纳米颗粒（NP）催化剂催化通常涉及复杂的级联反应步骤，但纳米颗粒对产物选择性的尺寸效应背后的机制尚未得到充分探讨。本文制备了一系列含镍分子筛催化剂，其中Ni纳米粒子均匀负载在H-ZSM-5分子筛的介孔和外表面。利用透射电子显微镜、原位x射线对分布函数和原位x射线吸收精细结构分析监测了Ni NPs在高分散Ni前驱体中的动态形成。通过控制还原温度，将金属纳米颗粒的粒径控制在3.72 ~ 11.91 nm之间。在间歇式反应器中，利用苯甲醛的还原胺化反应，对Ni NPs的低温催化性能进行了评价。这种反应本质上有利于形成一系列产物，但存在很大的选择性问题。我们的研究结果揭示了反应效率的大小依赖行为，催化剂在粒径为5.62(3)nm时达到最高的催化活性（93 %对伯胺的选择性）。这种最佳性能归因于氢化和胺化能力之间的平衡相互作用。这些发现突出了纳米颗粒尺寸与催化性能之间的复杂关系，强调了在催化剂设计中进行精确优化以提高工业应用中的选择性和可持续性的必要性。

{"title":"Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles","authors":"Yunong Li , Ching Kit Tommy Wun , Tianxiang Chen , Tsz Woon Benedict Lo","doi":"10.1016/j.mtcata.2025.100100","DOIUrl":"10.1016/j.mtcata.2025.100100","url":null,"abstract":"<div><div>Selectivity control is a fundamental focus in catalysis chemistry, as it directly reflects the efficiency and efficacy of catalytic processes. While catalysis often involves intricate and cascade reaction steps using nanoparticle (NP) catalysts, the mechanism behind the size effect of nanoparticles on product selectivity has not been fully explored. We herein prepared a series of Ni-containing zeolitic catalysts in which the Ni NPs are uniformly supported on the mesopores and outer surfaces of H-ZSM-5 zeolites. The dynamic formation of Ni NPs from highly dispersed Ni precursors was monitored using transmission electron microscopy, in-situ X-ray pair distribution function, and in-situ X-ray absorption fine structure analysis. The metal nanoparticle size was carefully controlled between 3.72(5) nm and 11.91(7) by controlling the reduction temperature. We evaluated the catalytic performance of Ni NPs using the reductive amination of benzaldehyde in batch reactors at low temperatures. This reaction inherently favors the formation of a series of products, suffering highly from selectivity issues. Our results revealed a size-dependent behavior in reaction efficiency, with the catalyst achieving the highest catalytic activity (93 % selectivity in primary amine) at a particle size of 5.62(3) nm. This optimal performance is attributed to a balanced interplay between hydrogenation and amination capabilities. These findings highlight the intricate relationship between nanoparticle size and catalytic performance, emphasizing the necessity for precise optimization in catalyst design to enhance selectivity and sustainability in industrial applications.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100100"},"PeriodicalIF":0.0,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143895821","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Assessing the photocatalytic activity of visible light active Bi2S3-based nanocomposites for Methylene Blue and Rhodamine B degradation 评价可见光活性bi2s3基纳米复合材料对亚甲基蓝和罗丹明B降解的光催化活性

Materials Today Catalysis

Pub Date : 2025-04-05 DOI: 10.1016/j.mtcata.2025.100099

Bachir Yaou Balarabe , Yerkanat N. Kanafin , Kuralay Rustembekkyzy , Imanzhussip Serkul , Meruert A. Nauryzbaeva , Timur Sh. Atabaev

High levels of organic compounds, notably synthetic dyes like Methylene blue (MB) and Rhodamine B (RhB), in untreated effluents have become a major environmental concern, endangering human health and ecosystems. These dyes are difficult to remove due to their non-biodegradable nature, prompting extensive research in this area. Photocatalysis has emerged as a promising, environmentally friendly method that only requires a light source and a photocatalyst for pollutant degradation. Bismuth sulfide (Bi₂S₃) stands out among other photocatalytic materials due to its narrow band gap, strong light absorption in the visible range, and nontoxicity, making it a good candidate to improve the overall photocatalytic efficiency. Therefore, this review article focuses on recent advances in Bi₂S₃-based nanocomposites and their role in the effective degradation of organic pollutants, particularly MB and RhB, through enhanced photocatalytic mechanisms.

在未经处理的废水中，高浓度的有机化合物，特别是合成染料，如亚甲基蓝（MB）和罗丹明B (RhB)，已成为一个主要的环境问题，危及人类健康和生态系统。这些染料由于其不可生物降解的性质而难以去除，这促使了该领域的广泛研究。光催化已经成为一种有前途的、环境友好的方法，它只需要一个光源和一个光催化剂就可以降解污染物。硫化铋（Bi2S3）具有窄带隙、可见光吸收强、无毒等特点，是提高整体光催化效率的理想材料。因此，本文主要综述了基于bi2s3的纳米复合材料的研究进展，以及它们通过增强光催化机制在有效降解有机污染物，特别是MB和RhB中的作用。

{"title":"Assessing the photocatalytic activity of visible light active Bi2S3-based nanocomposites for Methylene Blue and Rhodamine B degradation","authors":"Bachir Yaou Balarabe , Yerkanat N. Kanafin , Kuralay Rustembekkyzy , Imanzhussip Serkul , Meruert A. Nauryzbaeva , Timur Sh. Atabaev","doi":"10.1016/j.mtcata.2025.100099","DOIUrl":"10.1016/j.mtcata.2025.100099","url":null,"abstract":"<div><div>High levels of organic compounds, notably synthetic dyes like Methylene blue (MB) and Rhodamine B (RhB), in untreated effluents have become a major environmental concern, endangering human health and ecosystems. These dyes are difficult to remove due to their non-biodegradable nature, prompting extensive research in this area. Photocatalysis has emerged as a promising, environmentally friendly method that only requires a light source and a photocatalyst for pollutant degradation. Bismuth sulfide (Bi<sub>2</sub>S<sub>3</sub>) stands out among other photocatalytic materials due to its narrow band gap, strong light absorption in the visible range, and nontoxicity, making it a good candidate to improve the overall photocatalytic efficiency. Therefore, this review article focuses on recent advances in Bi<sub>2</sub>S<sub>3</sub>-based nanocomposites and their role in the effective degradation of organic pollutants, particularly MB and RhB, through enhanced photocatalytic mechanisms.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100099"},"PeriodicalIF":0.0,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143839610","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Constructing electron transport channel of SnO2/BaSO4 on g-C3N4 for enhanced visible-light-driven photocatalytic H2 production 在g-C3N4上构建SnO2/BaSO4的电子传递通道以增强可见光驱动光催化制氢

Materials Today Catalysis

Pub Date : 2025-03-24 DOI: 10.1016/j.mtcata.2025.100098

Gongyue Dong , Xiaojuan Guo , Cheng Cheng , Feng Chen , Jinfeng Zhang , Yanping Du , Wei Meng , Maochang Liu , Jinwen Shi

Graphitic carbon nitride (g-C₃N₄) is confronted with the issue of poor utilization of photogenerated charge carriers, thereby leading to limited performance of photocatalytic hydrogen (H₂) production, which restricts its potential application. Herein, the electron transport material SnO₂/BaSO₄ was synthesized to integrate with g-C₃N₄ for addressing the above problem. Various characterizations were conducted to investigate the g-C₃N₄-SnO₂/BaSO₄ photocatalyst, and it demonstrated that photogenerated electrons from g-C₃N₄ expeditiously migrate to SnO₂/BaSO₄ nanoparticles, which markedly hindered photogenerated carriers’ recombination. Subsequently, the g-C₃N₄-SnO₂/BaSO₄ photocatalyst demonstrated promoted photocatalytic H₂ production at a rate of 14.2 μmol h⁻¹ under visible-light illumination, which was 2.5 times higher than that of pristine g-C₃N₄.

石墨氮化碳（g-C3N4）面临光生载流子利用率差的问题，从而导致光催化制氢（H2）性能有限，限制了其潜在的应用前景。为了解决上述问题，本文合成了电子传输材料SnO2/BaSO4与g-C3N4集成。对g-C3N4-SnO2/BaSO4光催化剂进行了各种表征，结果表明，g-C3N4光生电子迅速迁移到SnO2/BaSO4纳米粒子上，这明显阻碍了光生载流子的重组。随后，g-C3N4- sno2 /BaSO4光催化剂在可见光照射下的光催化制氢速率为14.2 μmol h−1，是原始g-C3N4的2.5倍。

{"title":"Constructing electron transport channel of SnO2/BaSO4 on g-C3N4 for enhanced visible-light-driven photocatalytic H2 production","authors":"Gongyue Dong , Xiaojuan Guo , Cheng Cheng , Feng Chen , Jinfeng Zhang , Yanping Du , Wei Meng , Maochang Liu , Jinwen Shi","doi":"10.1016/j.mtcata.2025.100098","DOIUrl":"10.1016/j.mtcata.2025.100098","url":null,"abstract":"<div><div>Graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) is confronted with the issue of poor utilization of photogenerated charge carriers, thereby leading to limited performance of photocatalytic hydrogen (H<sub>2</sub>) production, which restricts its potential application. Herein, the electron transport material SnO<sub>2</sub>/BaSO<sub>4</sub> was synthesized to integrate with g-C<sub>3</sub>N<sub>4</sub> for addressing the above problem. Various characterizations were conducted to investigate the g-C<sub>3</sub>N<sub>4</sub>-SnO<sub>2</sub>/BaSO<sub>4</sub> photocatalyst, and it demonstrated that photogenerated electrons from g-C<sub>3</sub>N<sub>4</sub> expeditiously migrate to SnO<sub>2</sub>/BaSO<sub>4</sub> nanoparticles, which markedly hindered photogenerated carriers’ recombination. Subsequently, the g-C<sub>3</sub>N<sub>4</sub>-SnO<sub>2</sub>/BaSO<sub>4</sub> photocatalyst demonstrated promoted photocatalytic H<sub>2</sub> production at a rate of 14.2 μmol h<sup>−1</sup> under visible-light illumination, which was 2.5 times higher than that of pristine g-C<sub>3</sub>N<sub>4</sub>.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100098"},"PeriodicalIF":0.0,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143725196","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Improved low-temperature CO oxidation using heterogeneous nanofibrous structures decorated with Pd atoms and nanocrystals 用Pd原子和纳米晶体修饰的非均相纳米纤维结构改进低温CO氧化

Materials Today Catalysis

Pub Date : 2025-03-08 DOI: 10.1016/j.mtcata.2025.100093

M.A. Rodriguez-Olguin , D. Cazac , F. Ruiz-Zepeda , S. Bartling , M. Bosco , H. Atia , R. Eckelt , A. Manzo-Robledo , M. Vandichel , A. Aguirre , J.G.E. Gardeniers , A. Susarrey-Arce

Amorphous alumina shaped as nanofibers forming a non-woven network, functioning as a heterogeneous dispersion for palladium (Pd) atoms and nanocrystals, is unique yet unstudied for low-temperature CO oxidation. This work demonstrates that nanometric-size alumina fibers (ANFs) with a surface area of ⁓230 m²/g can host Pd species that remain nearly intact after CO oxidation. The ANFs contain various Pd (Pd-ANFs) loadings, ranging from 1 %wt. (Pd1-ANFs), 3 %wt. (Pd3-ANFs), to 5 %wt. (Pd5-ANFs). Among them, Pd3-ANFs show the highest CO chemisorption. Hence, the chemical environment of the Pd3-ANFs is assessed using NAP-XPS under various CO and O₂ mixtures. NAP-XPS shows the presence of metallic and oxidized Pd species. The results are correlated with DRIFT spectroscopy, which unveils the CO species adsorbed over Pd. Furthermore, a computational-based kinetic model for CO oxidation shows that Pd single atoms start the CO-oxidation, followed by larger Pd crystals during light-off. Our results demonstrate that the Pd-ANFs have higher activity when compared with the Pd alumina nanoparticles (Pd-ANP) counterpart that lacks a fibrous structure, highlighting the benefits of the ANF's structural network in stabilizing atomic and nanometric scale metal catalysts for low-temperature CO oxidation.

无定形氧化铝形状为纳米纤维，形成无纺布网络，作为钯（Pd）原子和纳米晶体的非均相分散体，是低温CO氧化的独特研究。这项工作表明，表面积为⁓230 m2/g的纳米级氧化铝纤维（ANFs）可以承载CO氧化后几乎保持完整的Pd物质。anf含有各种Pd （Pd- anf）负载，范围从1 %wt。 % wt (Pd1-ANFs) 3。（Pd3-ANFs），至5 %wt。(Pd5-ANFs)。其中，Pd3-ANFs表现出最高的CO化学吸附。因此，在不同CO和O2混合物下，使用NAP-XPS评估了Pd3-ANFs的化学环境。NAP-XPS显示金属态和氧化态钯的存在。结果与漂移光谱相关联，揭示了CO在Pd上的吸附。此外，基于计算的CO氧化动力学模型表明，Pd单原子开始CO氧化，随后在点燃过程中产生更大的Pd晶体。我们的研究结果表明，与缺乏纤维结构的Pd-氧化铝纳米颗粒（Pd- anp）相比，Pd-ANF具有更高的活性，突出了ANF结构网络在稳定原子和纳米级金属催化剂用于低温CO氧化方面的优势。

{"title":"Improved low-temperature CO oxidation using heterogeneous nanofibrous structures decorated with Pd atoms and nanocrystals","authors":"M.A. Rodriguez-Olguin , D. Cazac , F. Ruiz-Zepeda , S. Bartling , M. Bosco , H. Atia , R. Eckelt , A. Manzo-Robledo , M. Vandichel , A. Aguirre , J.G.E. Gardeniers , A. Susarrey-Arce","doi":"10.1016/j.mtcata.2025.100093","DOIUrl":"10.1016/j.mtcata.2025.100093","url":null,"abstract":"<div><div>Amorphous alumina shaped as nanofibers forming a non-woven network, functioning as a heterogeneous dispersion for palladium (Pd) atoms and nanocrystals, is unique yet unstudied for low-temperature CO oxidation. This work demonstrates that nanometric-size alumina fibers (ANFs) with a surface area of ⁓230 m<sup>2</sup>/g can host Pd species that remain nearly intact after CO oxidation. The ANFs contain various Pd (Pd-ANFs) loadings, ranging from 1 %wt. (Pd1-ANFs), 3 %wt. (Pd3-ANFs), to 5 %wt. (Pd5-ANFs). Among them, Pd3-ANFs show the highest CO chemisorption. Hence, the chemical environment of the Pd3-ANFs is assessed using NAP-XPS under various CO and O<sub>2</sub> mixtures. NAP-XPS shows the presence of metallic and oxidized Pd species. The results are correlated with DRIFT spectroscopy, which unveils the CO species adsorbed over Pd. Furthermore, a computational-based kinetic model for CO oxidation shows that Pd single atoms start the CO-oxidation, followed by larger Pd crystals during light-off. Our results demonstrate that the Pd-ANFs have higher activity when compared with the Pd alumina nanoparticles (Pd-ANP) counterpart that lacks a fibrous structure, highlighting the benefits of the ANF's structural network in stabilizing atomic and nanometric scale metal catalysts for low-temperature CO oxidation.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100093"},"PeriodicalIF":0.0,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629486","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0