Materials Today Catalysis最新文献

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Materials Today Catalysis

Pub Date : 2025-09-01 DOI: 10.1016/S2949-754X(25)00033-X

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Materials Today Catalysis

Pub Date : 2025-09-01 DOI: 10.1016/S2949-754X(25)00032-8

引用次数: 0

Thin-film approach for scalability and enhancement of solar hydrogen production with CNT integrated Ce-doped-TiO2 composite in direct sunlight 碳纳米管集成ce - tio2复合材料在阳光直射下的可扩展性和增强太阳能制氢的薄膜方法

Materials Today Catalysis

Pub Date : 2025-08-20 DOI: 10.1016/j.mtcata.2025.100115

Preethi Vijayarengan , Anthony Raja Maria , K.S. Ashadevi , Naresh Nalajala , Chinnakonda S. Gopinath

Solar hydrogen production by photocatalysis has long been considered as an important energy option. Whichever photocatalyst succeeds, methods should be available to scale-up in a most sustainable and cost-effective manner, and the present work addresses this specific issue. In the present study, Ce-doped in the TiO₂ lattice (Ce-TiO₂) and the same integrated with CNT (CNT-Ce-TiO₂; (CCT)) composite was synthesized and characterized. Current study demonstrates the synergistic integration of Ce-TiO₂ as a light absorber and charge generator with CNTs as efficient charge separation at heterojunctions as well as charge transporter in a thin-film configuration (lab-scale (4.7 cm²), bench-scale (500 cm²)). Improved H₂ generation under direct sunlight demonstrated in thin film form, than in particulate suspension, is attributed to efficient light absorption, particularly for electron-hole pair separation and their dispersion to redox sites. Additionally, the role of the binder is highlighted for improving H₂ yield and the sustainability of the thin-film form of photocatalyst. ∼200 mg (1 g) CCT coated over 500 cm² (2500 cm²) photocatalyst produced 21.6 mmol/h (102 mmol/h) H₂ in sunlight. Present results provides a proof of concept that the thin film form of photocatalyst displays, at least 10 times, higher H₂ yield than its powder counterpart, depending on the measurement conditions. A non-linear enhancement in H₂ yield with small and large area thin-film indicates complex underlying factors and highlights the scope for further improvements.

光催化太阳能制氢一直被认为是一种重要的能源选择。无论哪种光催化剂成功，都应该有方法以最可持续和最具成本效益的方式扩大规模，而目前的工作解决了这个具体问题。本研究合成并表征了ce掺杂在TiO2晶格中的（Ce-TiO2）和同样与CNT集成的（CNT-Ce-TiO2; (CCT)）复合材料。目前的研究证明了Ce-TiO₂作为光吸收剂和电荷发生器的协同集成，碳纳米管作为异质结的有效电荷分离以及薄膜结构中的电荷传输体（实验室规模（4.7 cm2），实验规模（500 cm2））。在阳光直射下，与颗粒悬浮液相比，薄膜形式的H2生成得到了改善，这归因于有效的光吸收，特别是电子-空穴对分离及其在氧化还原位点的分散。此外，还强调了粘合剂在提高H2产率和光催化剂薄膜形式的可持续性方面的作用。约200 mg（1 g）的CCT包被超过500 cm2（2500 cm2）的光催化剂在阳光下产生21.6 mmol/h（102 mmol/h）的H2。目前的结果提供了一个概念证明，薄膜形式的光催化剂显示，至少10倍高的H2产率比其粉末对应，取决于测量条件。小面积和大面积薄膜H2产率的非线性增强表明了复杂的潜在因素，并突出了进一步改进的空间。

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Construction of self-supporting heterobimetallic phosphides for oxygen evolution reaction 用于析氧反应的自支撑杂双金属磷化物的构建

Materials Today Catalysis

Pub Date : 2025-08-12 DOI: 10.1016/j.mtcata.2025.100114

Adjapong Linda Akua Agyapomaa , Chulong Jin , Qingqing Zhang, Xiaojun Zeng

Electrocatalysts with heterobimetallic active sites are considered to be effective geometries for electrocatalytic oxygen evolution reaction (OER). However, MOF-derived heterobimetallic phosphides are uncontrollable and the addition of traditional binders is complicated. Here, we designed an efficient defect-rich (NF/Ni₂P-Fe₂P@NC) heterostructure derived from NF/Fe-MOF, in which nickel foam (NF) provides a supporting role and Ni source to promote the formation of heterobimetallic phosphides (Ni₂P, Fe₂P). NF/Ni₂P-Fe₂P@NC inherits remarkable OER performance with ultralow overpotential of 123 mV at a current density of 10 mA cm⁻² and Tafel slope of 51. 3 mV dec⁻¹ in alkaline electrolyte. The experimental results unravel that the multi-components (Ni₂P, Fe₂P, NC), rich heterogeneous interfaces (Ni₂P/Fe₂P), and numerous defects in the heterostructure provide abundant active sites, optimize the electronic structure, and improve the exposure of active sites, thereby promoting the electrocatalytic OER process. Density functional theory (DFT) calculations confirm that the free energy barrier for the catalyst to generate *OOH intermediates is low. Our findings present a simple and economical approach to obtaining heterobimetallic phosphides with robust OER performance.

具有杂双金属活性位的电催化剂被认为是电催化析氧反应（OER）的有效结构。然而，mof衍生的杂双金属磷化物是不可控的，传统粘合剂的添加是复杂的。在此，我们设计了一种基于NF/Fe-MOF的高效富缺陷异质结构（NF/Ni2P-Fe2P@NC），其中泡沫镍（NF）提供了支撑作用和Ni源，以促进异双金属磷化物（Ni2P, Fe2P）的形成。NF/Ni2P-Fe2P@NC继承了卓越的OER性能，电流密度为10 mA cm−2，过电位为123 mV， Tafel斜率为51。3 mV dec−1在碱性电解质中。实验结果表明，多组分（Ni2P、Fe2P、NC）、丰富的异质界面（Ni2P/Fe2P）和众多的异质结构缺陷提供了丰富的活性位点，优化了电子结构，提高了活性位点的暴露，从而促进了电催化OER过程。密度泛函理论（DFT）计算证实，催化剂生成*OOH中间体的自由能垒较低。我们的发现提出了一种简单而经济的方法来获得具有强大OER性能的杂双金属磷化物。

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引用次数: 0

Comparative photoelectrochemical study of oligomeric s-heptazines nanomaterials derived from partial thermal decompositions of urea & thiourea precursors 尿素和硫脲前驱体部分热分解制备的低聚s-七嗪纳米材料的比较光电化学研究

Materials Today Catalysis

Pub Date : 2025-07-26 DOI: 10.1016/j.mtcata.2025.100112

Anupam Chowdhury , Dipanwita Majumdar , Moisilee Dutta , Swapan Kumar Bhattacharya

Thermal polymerization of urea and thiourea under closed conditions at 370 °C have been independently carried out and the derived samples were subjected to detailed characterization techniques that showed varied chemical compositions as well as distribution of functional groups despite the same C/N atomic ratio. The detailed optical, physicochemical and morphological characterizations from FTIR, RAMAN, XRD, TGA, XPS, solid-state & solution-state NMR, solid state UV–visible absorption, PL, BET, FESEM, TEM and SAED revealed that urea derived U370 sample with 2D flakes-like morphology closely resembles melem-cyanuric acid complex/adduct while thiourea derived T370 sample having flat ribbon-like structure can be intimately related with oligomeric melem (s-heptazines) hydrate respectively. Solution state UV–visible absorption spectroscopy, Zeta potential and Dynamic Light Scattering (DLS) aided size distribution studies were also conducted in aqueous media with varying pH to comprehend the character of chemical functionalities and nature of prevailing interactions in acid, neutral and alkaline electrolytes which were further be correlated with their photoelectrochemical responses. Their comparative electrochemical studies were conducted in aid with CV, GCD and EIS studies both under dark as well as in presence of different and wide range light sources in acid, neutral and basic media correspondingly to design low costing, eco-friendly, smart materials for light-driven supercapacitive devices. Results revealed T370 sample with better photoelectrochemical performance in terms of higher normalized areal capacitance, better rate capacity as well as improved cyclic stability than U370 sample in aqueous alkaline electrolyte. Thus, this communication outlines a novel approach for significantly upgrading the supercapacitive responses of materials using the simple aid of electromagnetic radiation, thereby opening up new roadways in the emerging field of photoelectrochemical charge storage and conversion technology.

在370 °C的封闭条件下，独立进行了尿素和硫脲的热聚合，并对衍生样品进行了详细的表征技术，尽管C/N原子比相同，但其化学成分和官能团分布却有所不同。通过FTIR、RAMAN、XRD、TGA、XPS、固态和固态等手段对材料进行了详细的光学、物理化学和形态表征；溶液态NMR、固相紫外可见吸收、PL、BET、FESEM、TEM和SAED分析表明，尿素衍生的U370样品具有二维片状结构，与melem-氰尿酸配合物/加合物非常相似，而硫脲衍生的T370样品具有扁平带状结构，与低聚物melem （s-七嗪）水合物密切相关。溶液状态紫外-可见吸收光谱、Zeta电位和动态光散射（DLS）辅助下的粒径分布研究也在不同pH的水介质中进行，以了解酸性、中性和碱性电解质的化学功能特征和主要相互作用的性质，并进一步与它们的光电化学反应相关联。他们在CV、GCD和EIS研究的辅助下进行了比较电化学研究，分别在黑暗和酸性、中性和碱性介质中不同范围的光源下进行，以设计低成本、环保、智能的光驱动超级电容器件材料。结果表明，与U370样品相比，T370样品在碱性水溶液中具有更高的归一化面积电容、更好的倍率容量和更好的循环稳定性。因此，本文概述了一种利用电磁辐射的简单辅助来显著提升材料超电容响应的新方法，从而在新兴的光电化学电荷存储和转换技术领域开辟了新的道路。

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引用次数: 0

La-doped and AgO-loading g-C3N4 heterojunctions for enhanced photocatalytic hydrogen evolution from water splitting la掺杂和ago负载的g-C3N4异质结增强光催化水裂解析氢

Materials Today Catalysis

Pub Date : 2025-07-25 DOI: 10.1016/j.mtcata.2025.100111

Hafiz Suleman Yaseen , Liu Deng , Li Luo , Johnny Muya Chabu , Syed Aamir Hussain , Wei Wang , Chengcheng Zhang , Rongrong Wang , Yifan Jiang , You-Nian Liu

Photocatalytic hydrogen evolution through water splitting represents a sustainable approach for green energy generation. Graphitic carbon nitride (g-C₃N₄)-based Z-scheme heterostructures have emerged as promising photocatalysts, but their practical applications are fundamentally limited by the persistent challenge of rapid charge recombination at heterointerfaces. To address this critical issue, we develop a novel Z-scheme photocatalyst AgO/La@g-C₃N₄ (ALCN) through integration of lanthanum-doped g-C₃N₄ nanosheets with AgO nanoparticles. Comprehensive structural analyses, optical characterization, and electrochemical evaluations confirm the successful construction of p-n heterojunctions with optimized band alignment. The engineered ALCN composite exhibits remarkable electron-hole separation efficiency, achieving an exceptional hydrogen production rate of 16.7 mmol g⁻¹ h⁻¹ under solar light irradiation, which represents a 13-fold, 4-fold, and 2-fold enhancement compared to pristine g-C₃N₄, La-doped g-C₃N₄, and the composite of La-doped g-C₃N₄ with Ag₂O counterparts, respectively. Mechanistic studies reveal that La-doping induces intermediate energy states facilitating charge migration, while the AgO/g-C₃N₄ heterojunction establishes directional Z-scheme charge transfer pathways. The optimized photocatalyst maintains 92 % activity after 5 cycles, demonstrating superior stability. This work establishes a new paradigm for designing efficient Z-scheme systems through synergistic metal loading and heterojunction engineering.

通过水裂解光催化析氢是一种可持续的绿色能源生产方法。基于石墨氮化碳（g-C3N4）的z型异质结构已经成为一种很有前途的光催化剂，但其实际应用从根本上受到异质界面快速电荷重组的持续挑战的限制。为了解决这一关键问题，我们通过将掺杂镧的g-C3N4纳米片与AgO纳米颗粒集成，开发了一种新型Z-scheme光催化剂AgO/La@g-C3N4 （ALCN）。综合结构分析、光学表征和电化学评价证实了p-n异质结的成功构建。经过改造的ALCN复合材料表现出了显著的电子空穴分离效率，在太阳光线照射下，其产氢率达到16.7 mmol g⁻¹ h⁻¹ ，与原始g- c3n4、la掺杂g- c3n4和la掺杂g- c3n4与Ag2O的复合材料相比，分别提高了13倍、4倍和2倍。机理研究表明，la掺杂诱导中间能态有利于电荷迁移，而AgO/g-C3N4异质结建立了定向Z-scheme电荷转移途径。优化后的光催化剂在5次循环后保持92 %的活性，表现出优异的稳定性。这项工作为通过协同金属加载和异质结工程设计高效的Z-scheme系统建立了一个新的范例。

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引用次数: 0

Advanced RuO2-based electrocatalysts for oxygen evolution reaction: A perspective from coordination structures 基于ruo2的先进析氧电催化剂：配位结构的视角

Materials Today Catalysis

Pub Date : 2025-07-11 DOI: 10.1016/j.mtcata.2025.100110

Qian Sun , Jiaxin Zhang , Wei Kong Pang , Bernt Johannessen , Peng Li , Guoqiang Zhao , Huaming Yang

Proton exchange membrane water electrolysis (PEMWE) is a promising technology for green hydrogen production, but its efficiency is limited by the sluggish oxygen evolution reaction (OER). RuO₂-based electrocatalysts exhibit superior intrinsic OER activity compared to IrO₂, yet their practical application is hindered by poor stability due to lattice oxygen overoxidation and Ru overoxidation. Recent advances highlight that modulating the local coordination environment of RuO₂ through doping, strain engineering, and defect control can not only optimize the OER pathways but also regulate the intrinsic activity of active sites, thereby achieving more balanced OER activity and stability. Meanwhile, computational investigations have also revealed deep insights into the catalytic performance of RuO₂ from the perspective of local coordination structures. Therefore, in this review, we start by discussing the OER mechanisms and common structural descriptors of the activity and stability of RuO₂. Then, we explore the relationship between structural regulation strategies and the OER performance of RuO₂ and analyze how coordination engineering influences catalytic behavior, establishing a designing framework for high-performance catalysts. Finally, we outline key challenges and future directions for RuO₂-based OER electrocatalysts in PEMWE applications.

质子交换膜水电解（PEMWE）是一种很有前途的绿色制氢技术，但其效率受到析氧反应（OER）缓慢的限制。与IrO2相比，基于ruo2的电催化剂具有更好的内在OER活性，但由于晶格氧过氧化和Ru过氧化，其稳定性较差，阻碍了其实际应用。近年来的研究表明，通过掺杂、应变工程和缺陷控制等手段调节RuO2的局部配位环境，不仅可以优化OER途径，还可以调节活性位点的内在活性，从而实现更平衡的OER活性和稳定性。同时，计算研究也从局部配位结构的角度深入了解了RuO2的催化性能。因此，在本文中，我们首先讨论了RuO2活性和稳定性的OER机制和常见的结构描述符。然后，我们探索了结构调控策略与RuO2 OER性能之间的关系，并分析了配位工程对催化行为的影响，建立了高性能催化剂的设计框架。最后，我们概述了基于ruo2的OER电催化剂在PEMWE应用中的主要挑战和未来方向。

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Recent advances in IB-group metal electrocatalysts for hydrogen conversion and utilization b族金属氢转化与利用电催化剂研究进展

Materials Today Catalysis

Pub Date : 2025-07-04 DOI: 10.1016/j.mtcata.2025.100109

Wen-Xuan Lv , Kai-Xuan Jiang , Yue-Bao Chen , Peng-Fei Yin , Hui Liu , Xi-Wen Du

The green production, conversion, and utilization of hydrogen energy rely heavily on key technologies such as water electrolysis and hydrogen fuel cells. As essential components of these technologies, metal catalysts play a crucial role in determining device efficiency and economic viability. Currently, most electrocatalysts still rely on noble metals; however, their high cost and resource scarcity severely limit large-scale application and commercialization. Therefore, the development of cost-effective and high-performance alternatives to noble metal catalysts has become a major research focus. IB-group metals (Cu, Ag) have emerged as promising candidates for electrocatalysis due to their low cost, high electrical conductivity, and excellent corrosion resistance. However, their d¹⁰ electronic configuration results in weak adsorption of catalytic intermediates, leading to inherently low catalytic activity. Over the past decade, advancements in synthesis techniques and atomic/electronic structure modulation strategies have enabled the transformation of IB-group metals, particularly Cu and Ag, into highly efficient electrocatalysts for the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). This review systematically summarizes recent progress in the synthesis and structural optimization of IB-group metal catalysts, with a particular focus on their applications in water electrolysis and hydrogen fuel cells. By analyzing key factors such as crystal structure and electronic configuration, we elucidate the fundamental mechanisms influencing catalytic performance. Finally, we discuss future perspectives on IB-group metal catalysts in clean energy technologies, highlighting their potential to accelerate the development of hydrogen energy and contribute to global carbon neutrality goals.

氢能源的绿色生产、转化和利用在很大程度上依赖于水电解和氢燃料电池等关键技术。作为这些技术的重要组成部分，金属催化剂在决定设备效率和经济可行性方面起着至关重要的作用。目前，大多数电催化剂仍然依赖于贵金属；然而，它们的高成本和资源稀缺性严重限制了它们的大规模应用和商业化。因此，开发具有成本效益和高性能的贵金属催化剂替代品已成为一个重要的研究热点。b族金属（Cu, Ag）由于其低成本、高导电性和优异的耐腐蚀性而成为电催化的有希望的候选者。然而，它们的d10电子结构导致催化中间体的吸附弱，导致固有的低催化活性。在过去的十年中，合成技术和原子/电子结构调制策略的进步使ib族金属，特别是Cu和Ag，成为析氢反应（HER）和氧还原反应（ORR）的高效电催化剂。本文系统地综述了ib族金属催化剂的合成和结构优化的最新进展，重点介绍了ib族金属催化剂在水电解和氢燃料电池中的应用。通过对晶体结构和电子构型等关键因素的分析，阐明了影响催化性能的基本机理。最后，我们讨论了b族金属催化剂在清洁能源技术中的未来前景，强调了它们在加速氢能源发展和促进全球碳中和目标方面的潜力。

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Ediorial Board Ediorial董事会

Materials Today Catalysis

Pub Date : 2025-06-01 DOI: 10.1016/S2949-754X(25)00021-3

引用次数: 0

Allying cobalt nanoclusters with carbon nanofibers for selectively electrocatalytic hydrogenation of unsaturated aldehyde with water as hydrogen source 以水为氢源，钴纳米团簇与碳纳米纤维选择性电催化不饱和醛加氢

Materials Today Catalysis

Pub Date : 2025-06-01 DOI: 10.1016/j.mtcata.2025.100104

Xinyu Yang , Sheng-Hua Zhou , Xiaofang Li , Xin-Tao Wu , Qi-Long Zhu

The electrocatalytic hydrogenation of α, β-unsaturated aldehydes has attracted significant attention, yet the design of electrocatalysts with selective adsorption over CC or CO bond remaining a challenging task. In this study, the Co nanoclusters anchored onto the nitrogen-doped porous carbon nanofibers were elaborately fabricated for efficient electrocatalytic hydrogenation. A kinetically driven mono-micelle-oriented self-assembly method was applied to synthesize the polymer nanofibers as the accommodation for Co^2 +. The stepwise pyrolysis of Co²⁺/polymer nanofibers with dicyandiamide yielded the evenly distributed Co nanoclusters with an average size of ∼4 nm over the nitrogen-doped porous carbon nanofibers. Benefited from the high activity of the Co nanoclusters and their rapid electron communication with the nitrogen-doped porous carbon nanofibers, this electrocatalyst demonstrated excellent performance in the selectively electrocatalytic hydrogenation of cinnamaldehyde to hydrocinnamaldehyde, achieving a high selectivity of 90.9 % and a conversion of 68.2 % at 12 mA cm⁻². The further in-situ spectroscopy analysis and density functional theory calculations revealed the more preferred adsorption of CC bond and easier water dissociation to give the active H atoms over the Co nanoclusters, which shed light on the hydrogenation mechanism over this electrocatalyst. Our study can provide a new insight in catalyst design for electrocatalytic hydrogenation reaction.

α， β-不饱和醛的电催化加氢已经引起了人们的广泛关注，但在CC键或CO键上选择性吸附的电催化剂的设计仍然是一个具有挑战性的任务。在这项研究中，Co纳米团簇固定在氮掺杂的多孔碳纳米纤维上，用于高效的电催化加氢。采用动力学驱动的单胶束定向自组装方法合成了聚合物纳米纤维，作为Co2 +的容纳体。用双氰胺对Co2+/聚合物纳米纤维进行分步热解，得到了均匀分布的Co纳米团簇，平均尺寸为~ 4 nm。得益于Co纳米团簇的高活性及其与氮掺杂多孔碳纳米纤维的快速电子通信，该电催化剂在选择性电催化肉桂醛加氢为氢肉桂醛方面表现出了优异的性能，在12 mA cm−2下达到了90.9 %的高选择性和68.2% %的转化率。进一步的原位光谱分析和密度泛函理论计算表明，与Co纳米团簇相比，CC键更容易吸附，水解离更容易产生活性H原子，从而揭示了该电催化剂的加氢机理。本研究为电催化加氢反应的催化剂设计提供了新的思路。

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