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Catalytic Mechanism Studies of Ortho–para H2 Conversion Over Iron Oxide Catalysts 氧化铁催化剂催化邻位对位H2转化机理研究
Pub Date : 2025-04-21 DOI: 10.1002/ece2.70004
Yusen Chen, Hongying Zhuo, Zheng Shen, Nan Yin, Zhongzheng Zhao, Binglian Liang, Guodong Liu, Xuning Li, Xiaofeng Yang, Yanqiang Huang

Hydrogen serves as an ideal clean energy with zero carbon emissions, whereas its large-scale application relies on its liquidation, by which the catalytic conversion of ortho–para H2 at cryogenic temperature is inevitable with iron oxides as a promising catalyst. In this research, iron oxides with varied surface area and diverse phases were synthesized from the precursor of hydrous ferric oxide, including α-Fe2O3, γ-Fe2O3, and Fe3O4. The bulk and surface properties of these catalysts were characterized by XRD, BET, TG, IR, magnetic analysis, hydrogen adsorption, and 57Fe-Mössbauer spectrum. It was suggested that ortho–para H2 conversion is linearly correlated with the specific surface area of α-Fe2O3 which governs the residual magnetic properties as well as the adsorption capacity of molecular H2 on the catalysts, and a nondissociation mechanism of ortho–para H2 conversion was revealed at cryogenic temperature. The hydrate that contributed to the surface area of iron oxides shows a negative effect on the ortho–para H2 conversion. Moreover, by estimating the reaction rate based on the per surface area of iron oxides, the Fe(III) exposed on surfaces exhibited a superior activity irrespective of the bulk magnetism of iron oxides, and the intrinsic activity of iron oxides for ortho–para H2 conversion was found to follow a trend similar to that of α-Fe2O3γ-Fe2O3 > Fe3O4. The findings of this study provide valuable insights for the subsequent research on the mechanism of ortho–para H2 conversion and the design of high-performance hydrogen liquefaction catalysts.

氢是一种理想的零碳排放清洁能源,但它的大规模应用依赖于它的清算,而氧化铁作为一种有前景的催化剂,在低温下催化转化正对H2是不可避免的。本研究以水合氧化铁前驱体α-Fe2O3、γ-Fe2O3和Fe3O4为原料,合成了不同相、不同表面积的氧化铁。采用XRD、BET、TG、IR、磁分析、氢吸附和57Fe-Mössbauer谱对催化剂的体积和表面性能进行了表征。结果表明,α-Fe2O3的比表面积决定了催化剂的剩余磁性能和H2分子在催化剂上的吸附能力,并揭示了低温下邻对H2转化的非解离机理。对氧化铁表面积有贡献的水合物对邻对H2转化有负影响。此外,根据氧化铁的单位表面积估算反应速率,发现暴露在表面的Fe(III)表现出优越的活性,而与氧化铁的体磁性无关,并且发现氧化铁的邻对H2转化的本构活性遵循与α-Fe2O3≈γ-Fe2O3 >; Fe3O4相似的趋势。本研究结果为后续对邻对氢转化机理的研究和高性能氢液化催化剂的设计提供了有价值的见解。
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引用次数: 0
Titanium-Doped Hematite Homojunction Photoanodes Based on Nanorod/Nanobowl Arrays for Efficient Solar Water Splitting 基于纳米棒/纳米碗阵列的掺钛赤铁矿均匀结光阳极用于高效太阳能水分解
Pub Date : 2025-04-18 DOI: 10.1002/ece2.70005
Kexin Ren, Zihao Wu, Simin Zhang, Limin Qi

Hematite is a promising candidate material for photoanodes, but the efficiency of the state-of-the-art hematite photoanodes is limited by the low absorption coefficient, short hole diffusion length, and slow water oxidation kinetics. In this work, a high-efficiency hematite photoanode was designed and fabricated by introducing titanium-doped hematite (Ti:Fe2O3) homojunction with different doping contents and a hierarchical nanorod/nanobowl array structure. The homojuction consisted of low Ti doping nanorods grown on high Ti doping nanobowl arrays, leading to the formation of a broad built-in electric field, significantly enhancing the charge separation and transfer within the bulk. Furthermore, the nanorods radially grown inside the bowls and on the bowl edges enabled enhanced light absorption through multiple light scattering while offering a larger electrode–electrolyte contact area and providing more reaction sites. Compared to the Ti:Fe2O3 nanorod arrays, the Ti:Fe2O3 nanorod/nanobowl array photoanode exhibited an increase in photocurrent density from 1.6 mA cm−2 to 3.0 mA cm−2 at 1.23 V versus RHE, maintaining long-term stability over 100 h at 1.23 V versus RHE. This study not only achieved a high-performance hematite photoanode but also provided a new perspective on the design of differently doping homojunction photoanodes with desired nanostructures.

赤铁矿是一种很有前途的光阳极候选材料,但目前最先进的赤铁矿光阳极的效率受到吸收系数低、孔扩散长度短和水氧化动力学慢的限制。本研究通过引入不同掺杂量的掺钛赤铁矿(Ti:Fe2O3)均结和层叠纳米棒/纳米碗阵列结构,设计并制备了高效赤铁矿光阳极。低钛掺杂的纳米棒生长在高钛掺杂的纳米碗阵列上,形成了广阔的内置电场,显著增强了体内电荷的分离和转移。此外,纳米棒径向生长在碗内和碗边缘,通过多次光散射增强光吸收,同时提供更大的电极-电解质接触面积和更多的反应位点。与Ti:Fe2O3纳米棒阵列相比,Ti:Fe2O3纳米棒/纳米碗阵列光阳极在1.23 V / RHE下的光电流密度从1.6 mA cm - 2增加到3.0 mA cm - 2,在1.23 V / RHE下保持100小时的长期稳定性。本研究不仅实现了高性能赤铁矿光阳极,而且为设计不同掺杂的纳米结构的均结光阳极提供了新的视角。
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引用次数: 0
Fabricating α-MnO2@NiMoO4 Heterostructure Architecture With Superior Photoelectrocatalytic Water Purification 利用优越的光电催化水净化技术制备α-MnO2@NiMoO4异质结构
Pub Date : 2025-04-08 DOI: 10.1002/ece2.70003
Hongchao Ma, Yan Chen, Huijun Li, Yinghuan Fu, Dedong Sun, Guowen Wang, Xiang Guo, Shixue Dou, Vadivel Subramaniam, Ashish Kumar, Krishnamoorthy Ramachandran, Xinghui Liu

Heterostructure catalyst is highly efficient for photoelectrolytic (PEC) wastewater remediation, while rationally constructing the photoelectrocatalyst with a high-quality interface is still challenging. Herein, a simple hydrothermal process prepares a heterostructure NiMoO4@α-MnO2 with a uniform interface between NiMoO4 nanosheets and α-MnO2 nanowires. NiMoO4@α-MnO2 exhibited significant advantages as follows: (1) α-MnO2 nanowires act as charge transport channels like the arteries that transport nutrients, promoting the migration and separation of induced charges; (2) the pollutants can be electrostatically concentrated to the surface of the NiMoO4@α-MnO2. Specifically, the gossamer-like NiMoO4 nanosheets adhering on the surface of the α-MnO2 have a large surface area, beneficial for electrolyte penetration and utilization of active sites. (3) Unfolded gossamer-like NiMoO4, like a vast extended solar panel of an artificial satellite, can harvest more solar energy, generating lots of electron (e)/hole (h+) pairs and active species, offering multiple transfer pathways and speeding up the rate of the degradation reaction. The optimized heterostructured NiMoO4@α-MnO2-3.5 catalysts showed superior PEC activity and remarkable stability for degrading reactive brilliant blue KN-R. Z-scheme heterojunction between α-MnO2 and NiMoO4 is proposed based on their energy band structure and free radical quenching experiment.

异质结构催化剂是光解废水高效修复的催化剂,但合理构建具有高质量界面的光电催化剂仍是一个挑战。本文采用简单的水热法制备了具有NiMoO4纳米片与α-MnO2纳米线界面均匀的异质结构NiMoO4@α-MnO2。NiMoO4@α-MnO2表现出如下显著优势:(1)α-MnO2纳米线像输送营养物质的动脉一样充当电荷输送通道,促进诱导电荷的迁移和分离;(2)污染物可以静电富集到NiMoO4@α-MnO2表面。具体来说,附着在α-MnO2表面的蛛丝状NiMoO4纳米片具有较大的表面积,有利于电解质的渗透和活性位点的利用。(3)展开后的蛛丝状NiMoO4,就像人造卫星上一个巨大的扩展太阳能电池板,可以收集更多的太阳能,产生大量的电子(e−)/空穴(h+)对和活性物质,提供了多种传递途径,加快了降解反应的速度。优化后的异质结构NiMoO4@α-MnO2-3.5催化剂具有优异的PEC活性和降解活性艳蓝KN-R的稳定性。根据α-MnO2和NiMoO4的能带结构和自由基猝灭实验,提出了α-MnO2和NiMoO4之间的z型异质结。
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引用次数: 0
Multiple Hydrogen-Bond Cross-Linking Solid–Solid Phase Change Materials for Batteries’ Thermal Management 多氢键交联固固相变材料在电池热管理中的应用
Pub Date : 2025-03-22 DOI: 10.1002/ece2.70002
Xuemei Diao, Peng Wang, Yang Li, Xiao Chen

Solid–solid phase change materials usually suffer from the challenges of low thermal storage capacity and poor mechanical strength in thermal management applications. Additionally, solid–solid phase change materials are often prepared by a chemical cross-linking strategy, leading to poor recyclability. This study highlights a straightforward and effective strategy to prepare multiple H-bonding cross-linking supramolecular solid–solid phase change materials integrating easy recyclability, high mechanical strength, and high latent heat characteristics for thermal management of lithium batteries.

固-固相变材料在热管理应用中通常面临储热能力低和机械强度差的挑战。此外,固-固相变材料通常采用化学交联策略制备,导致可回收性差。本研究为锂电池热管理提供了一种简单有效的策略来制备具有易于回收、高机械强度和高潜热特性的多h键交联超分子固-固相变材料。
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引用次数: 0
Challenges and Opportunities in the Use of Iron Photosensitizers for Dye-Sensitized Solar Cells and Photoelectrosynthetic Cells Applications 铁光敏剂在染料敏化太阳能电池和光电合成电池应用中的挑战与机遇
Pub Date : 2025-03-09 DOI: 10.1002/ece2.70001
Lakshmi Narayan Satheesh, Katerina Achilleos, Abdullah M. Abudayyeh, Ludovic Troian-Gautier

Novel renewable alternatives to meet the needs of our current energy landscape are highly sought after. Photovoltaic solar cells (PV) are considered leading candidates for carbon neutrality due to their numerous benefits and good solar-to-energy conversion efficiency. However, the need is no longer solely focused on electric current generation but also on strategies to store that energy. This led, amongst other technologies, to the development of dye-sensitized photoelectrosynthesis cells (DSPECs), the successor of dye-sensitized solar cells (DSSCs). However, these cost-effective solar cells mostly use photosensitizers based on scarce metals such as ruthenium. Iron-based photosensitizers represent the holy grail due to their low toxicity, greater abundance, and versatile chemistry. However, they still suffer from drastic limitations: their photochemistry and extremely fast excited-state deactivation processes lead to inefficient charge injection and/or fast charge recombination. This review gathers examples of iron-based photosensitizers that have been successfully immobilized on metal oxide surfaces. A critical comparison of Fe-based photosensitizers is made based on their photophysical properties, electrochemistry, and photovoltaic performances.

新颖的可再生能源替代品,以满足我们当前的能源格局的需求是备受追捧的。光伏太阳能电池(PV)由于其众多优点和良好的太阳能-能源转换效率而被认为是碳中和的主要候选者。然而,需求不再仅仅集中在发电上,而且还集中在储存能量的策略上。在其他技术中,这导致了染料敏化光电合成电池(DSPECs)的发展,染料敏化太阳能电池(DSSCs)的继承者。然而,这些具有成本效益的太阳能电池大多使用基于稀有金属(如钌)的光敏剂。铁基光敏剂因其毒性低、丰度高和化学用途广泛而成为人们追求的目标。然而,它们仍然受到严重的限制:它们的光化学和极快的激发态失活过程导致低效的电荷注入和/或快速电荷重组。本文综述了铁基光敏剂已成功固定在金属氧化物表面的例子。基于铁基光敏剂的光物理性能、电化学性能和光伏性能,对其进行了关键的比较。
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引用次数: 0
Biomass-Derived Carbon and Their Composites for Supercapacitor Applications: Sources, Functions, and Mechanisms 生物质衍生碳及其复合材料在超级电容器中的应用:来源、功能和机制
Pub Date : 2025-03-04 DOI: 10.1002/ece2.70000
Xi Zhu, Yi Zeng, Xianhui Zhao, Dan Liu, Weiwei Lei, Shun Lu

Biomass-derived carbons are eco-friendly and sustainable materials, making them ideal for supercapacitors due to their high surface area, excellent conductivity, cost-effectiveness, and environmental benefits. This review provides valuable insights into biomass-derived carbon and modified carbon for supercapacitors, integrating both experimental results and theoretical calculations. This review begins by discussing the origins of biomass-derived carbon in supercapacitors, including plant-based, food waste-derived, animal-origin, and microorganism-generated sources. Then, this review presents strategies to improve the performance of biomass-derived carbon in supercapacitors, including heteroatom doping, surface functionalization, and hybrid composite construction. Furthermore, this review analyzes the functions of biomass-derived carbon in supercapacitors both in its pure form and as modified materials. The review also explores composites derived from biomass-based carbon, including carbon/MXenes, carbon/MOFs, carbon/graphene, carbon/conductive polymers, carbon/transition metal oxides, and carbon/hydroxides, providing a thorough investigation. Most importantly, this review offers an innovative summary and analysis of the role of biomass-derived carbon in supercapacitors through theoretical calculations, concentrating on four key aspects: energy band structure, density of states, electron cloud density, and adsorption energy. Finally, the review concludes the future research directions for biomass carbon-based supercapacitors, including the discovery of novel biomass materials, tailoring surface functional groups, fabricating high-performance composite materials, exploring ion transfer mechanisms, and enhancing practical applications. In summary, this review offers a thorough exploration of the sources, functions, and mechanisms of biomass-derived carbon in supercapacitors, providing valuable insights for future research.

生物质衍生的碳是环保和可持续的材料,由于其高表面积,优异的导电性,成本效益和环境效益,使其成为超级电容器的理想选择。本文结合实验结果和理论计算,对生物质碳和改性碳在超级电容器中的应用提供了有价值的见解。本文首先讨论了超级电容器中生物质来源的碳的来源,包括植物来源、食物垃圾来源、动物来源和微生物来源。然后,本文综述了提高生物质碳超级电容器性能的策略,包括杂原子掺杂、表面功能化和杂化复合材料的构建。此外,本文还分析了生物质碳在超级电容器中的纯形式和改性材料的功能。该综述还探讨了由生物质碳衍生的复合材料,包括碳/MXenes、碳/ mof、碳/石墨烯、碳/导电聚合物、碳/过渡金属氧化物和碳/氢氧化物,提供了全面的研究。最重要的是,本文通过理论计算对生物质碳在超级电容器中的作用进行了创新性的总结和分析,重点关注了四个关键方面:能带结构、态密度、电子云密度和吸附能。最后,总结了生物质碳基超级电容器未来的研究方向,包括发现新型生物质材料、定制表面官能团、制备高性能复合材料、探索离子转移机制、加强实际应用等。综上所述,本文对超级电容器中生物质碳的来源、功能和机制进行了深入的探索,为未来的研究提供了有价值的见解。
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引用次数: 0
Insights Into the Light-Driven Conversion of Methane: Mechanisms, Characterization, and Perspective 洞察甲烷的光驱动转换:机制,表征和观点
Pub Date : 2025-02-26 DOI: 10.1002/ece2.96
Jiayi Chen, Shiqin Gao, Tao Gan, Bolun Wang

Methane, recognized as a promising substitute for conventional fossil fuels due to its abundant availability, low cost, and high energy density, can be converted into value-added products, providing a sustainable energy–carbon utilization approach. However, its inert molecules require significant energy for C–H bond activation. Photocatalytic conversion offers an effective mild-condition solution, reducing thermocatalysis energy demands and enhancing activation efficiency for selective chemical production. This review systematically arranges photocatalytic C–H bond activation mechanisms, categorizes conversion products, and discusses challenges, prospects, and solutions for methane photocatalysis development.

甲烷由于其丰富的可用性、低成本和高能量密度而被公认为传统化石燃料的有前途的替代品,可以转化为增值产品,提供了一种可持续的能源-碳利用方法。然而,它的惰性分子需要大量的能量来激活C-H键。光催化转化提供了一种有效的温和条件解决方案,减少了热催化能量需求,提高了选择性化学生产的激活效率。本文系统梳理了光催化C-H键活化机理,对转化产物进行了分类,并对甲烷光催化发展面临的挑战、前景和解决方案进行了讨论。
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引用次数: 0
Insights into the roles of natural graphite in phase change materials 天然石墨在相变材料中的作用
Pub Date : 2025-02-16 DOI: 10.1002/ece2.93
Zhaodi Tang, Dongmei Huang, Xi Zhang, Bin Wang, Sidong Yu, Ruoyu Guo, Qimin Sun, Jionghui Wang

Phase change materials (PCMs) that reversibly release or absorb thermal energy during phase transitions play a significant role in promoting renewable and sustainable energy development. However, the poor shape stability, low thermal conductivity, and inferior energy conversion efficiency of PCMs hinder their wider applicability and are difficult to meet the growing demand. As the precursor of carbon-based materials, including expanded graphite, graphene oxide, and graphene, natural graphite (NG) finds extensive applications and bring new potentials to the PCMs, enabling multiple cutting-edge thermal energy applications. Herein, we systematically discuss NG and its derivative-based composite PCMs for thermal energy storage, thermal energy conduction, and thermal energy conversion. This paper aims to offer insights into the roles of NG in PCMs and hope to provide a useful guide for the design of next-generation composite PCMs with high-energy-density, high thermal conductivity and high energy conversion efficiency.

相变材料在相变过程中可逆地释放或吸收热能,对促进可再生能源和可持续能源的发展具有重要作用。然而,pcm的形状稳定性差、导热系数低、能量转换效率低等缺点阻碍了其更广泛的应用,难以满足日益增长的需求。作为膨胀石墨、氧化石墨烯和石墨烯等碳基材料的前体,天然石墨(NG)具有广泛的应用前景,并为pcm带来了新的潜力,实现了多种尖端热能应用。在此,我们系统地讨论了基于天然气及其衍生物的复合相变材料的热能储存,热能传导和热能转换。本文旨在深入探讨ngm在pcm中的作用,希望为下一代高能量密度、高导热、高能量转换效率的复合pcm的设计提供有益的指导。
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引用次数: 0
Solvation chemistry in liquid electrolytes for rechargeable lithium batteries at low temperatures 低温下可充电锂电池液体电解质的溶剂化化学
Pub Date : 2025-02-12 DOI: 10.1002/ece2.94
Houzhen Li, Chuncheng Yan, Shuhua Wang

Over the past few decades, significant advancements have been made in the development of low-temperature liquid electrolytes for lithium batteries (LBs). Ongoing exploration of liquid electrolytes is crucial for further enhancing the performance of these batteries. Solvation chemistry plays a dominant role in determining the properties of the electrolyte, significantly affecting LBs performance at low temperatures (LTs). This review introduces solvation structures and their impact, discussing how these structures promote fast desolvation processes and contribute to the improvement of battery performance. Additionally, various solvent strategies are highlighted to refine solvation chemistry at LTs, including the use of linear and cyclic ethers/esters, as well as the role of functional groups within these solvents. The review also summarizes the impact of lithium salts containing organic/inorganic anions on solvation chemistry. Characterization techniques for solvent chemistry are discussed, providing a comprehensive analysis that offers valuable insights for developing next-generation electrolytes to ensure reliable battery performance across a wide temperature range.

在过去的几十年里,锂电池低温液体电解质的研究取得了重大进展。对液体电解质的持续探索对于进一步提高这些电池的性能至关重要。溶剂化化学在电解质的性质中起着主导作用,显著影响着lb在低温下的性能。本文介绍了溶剂化结构及其影响,讨论了这些结构如何促进快速脱溶过程并有助于提高电池性能。此外,还强调了各种溶剂策略,以改进LTs的溶剂化化学,包括线性和环醚/酯的使用,以及官能团在这些溶剂中的作用。综述了含有机/无机阴离子锂盐对溶剂化化学的影响。讨论了溶剂化学表征技术,提供了一个全面的分析,为开发下一代电解质提供了有价值的见解,以确保在广泛的温度范围内可靠的电池性能。
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引用次数: 0
Structural and electronic double effects on S-doping dendritic mesoporous CeFeW/DM catalyst for enhancing SO2 tolerance in the low temperature NH3-SCR reaction s掺杂枝状介孔CeFeW/DM催化剂在NH3-SCR低温反应中增强SO2耐受性的结构和电子双效应
Pub Date : 2025-02-10 DOI: 10.1002/ece2.95
Xiaosheng Huang, Weitong Ling, Rongji Cui, Xiaona Li, Yongjie Xi, Zhicheng Tang

SO2 poisoning severely impedes the development of Ce-based catalysts in NH3-SCR process for nitrogen oxides elimination. S-doping dendritic mesoporous

(DM)-structured CeFeW/DM catalyst has been carefully designed in this work and its tolerance to SO2 has been effectively enhanced. The DM structure allowed metal oxides to be highly dispersed and generated Ce–O–Fe active pairs with enhancing redox ability via the efficient electron transfer between Ce3+ + Fe3+ ↔ Ce4+ + Fe2+. Importantly, the opened center–radial pore channels not only facilitated rapid adsorption of NO and NH3, but also distinctly alleviated the problem of ammonium sulfate blocking the catalyst pores during the NH3-SCR process. Notably, S-doping enhanced the surface acidity and inhibited the adsorption and oxidation of SO2 effectively. Besides, density functional theory calculation revealed that S-doping further perturbed the local electronic environment and formed an electron enrichment region around the Ce–O–Fe interface, which made SO2 preferentially adsorbed on Fe sites, whereas NO was more inclined to be adsorbed on Ce sites. Therefore, the Ce active site was protected from SO2 poisoning, enabling both L-H and E-R reaction pathways simultaneously occurring with smooth adsorption and activation of NO on CeFeW/DM. This study deeply reveals the coordination efforts between catalyst structure and electronic effects, which provided a new idea for designing highly efficient SO2-resistant Ce-based catalysts for low temperature NH3-SCR reaction.

在NH3-SCR工艺中,SO2中毒严重阻碍了ce基催化剂的发展。本研究精心设计了s掺杂枝晶介孔(DM)结构的CeFeW/DM催化剂,有效提高了其对SO2的耐受性。DM结构允许金属氧化物高度分散,并通过Ce3+ + Fe3+之间有效的电子转移产生Ce-O-Fe活性对,从而增强了Ce3+ + Fe3+之间的氧化还原能力。重要的是,打开的中心-径向孔通道不仅促进了NO和NH3的快速吸附,而且明显缓解了NH3- scr过程中硫酸铵堵塞催化剂孔的问题。值得注意的是,s掺杂提高了表面酸度,有效地抑制了SO2的吸附和氧化。此外,密度泛函理论计算表明,s掺杂进一步扰动了局部电子环境,在Ce - o - Fe界面周围形成了电子富集区,使得SO2优先吸附在Fe位点上,而NO更倾向于吸附在Ce位点上。因此,Ce活性位点免受SO2毒害,使L-H和E-R反应途径同时发生,并在CeFeW/DM上顺利吸附和激活NO。该研究深入揭示了催化剂结构与电子效应之间的协同作用,为设计高效耐so2低温NH3-SCR反应ce基催化剂提供了新的思路。
{"title":"Structural and electronic double effects on S-doping dendritic mesoporous CeFeW/DM catalyst for enhancing SO2 tolerance in the low temperature NH3-SCR reaction","authors":"Xiaosheng Huang,&nbsp;Weitong Ling,&nbsp;Rongji Cui,&nbsp;Xiaona Li,&nbsp;Yongjie Xi,&nbsp;Zhicheng Tang","doi":"10.1002/ece2.95","DOIUrl":"https://doi.org/10.1002/ece2.95","url":null,"abstract":"<div>\u0000 \u0000 \u0000 <section>\u0000 \u0000 <p>SO<sub>2</sub> poisoning severely impedes the development of Ce-based catalysts in NH<sub>3</sub>-SCR process for nitrogen oxides elimination. S-doping dendritic mesoporous</p>\u0000 \u0000 <p>(DM)-structured CeFeW/DM catalyst has been carefully designed in this work and its tolerance to SO<sub>2</sub> has been effectively enhanced. The DM structure allowed metal oxides to be highly dispersed and generated Ce–O–Fe active pairs with enhancing redox ability via the efficient electron transfer between Ce<sup>3+</sup> + Fe<sup>3+</sup> ↔ Ce<sup>4+</sup> + Fe<sup>2+</sup>. Importantly, the opened center–radial pore channels not only facilitated rapid adsorption of NO and NH<sub>3</sub>, but also distinctly alleviated the problem of ammonium sulfate blocking the catalyst pores during the NH<sub>3</sub>-SCR process. Notably, S-doping enhanced the surface acidity and inhibited the adsorption and oxidation of SO<sub>2</sub> effectively. Besides, density functional theory calculation revealed that S-doping further perturbed the local electronic environment and formed an electron enrichment region around the Ce–O–Fe interface, which made SO<sub>2</sub> preferentially adsorbed on Fe sites, whereas NO was more inclined to be adsorbed on Ce sites. Therefore, the Ce active site was protected from SO<sub>2</sub> poisoning, enabling both L-H and E-R reaction pathways simultaneously occurring with smooth adsorption and activation of NO on CeFeW/DM. This study deeply reveals the coordination efforts between catalyst structure and electronic effects, which provided a new idea for designing highly efficient SO<sub>2</sub>-resistant Ce-based catalysts for low temperature NH<sub>3</sub>-SCR reaction.</p>\u0000 </section>\u0000 </div>","PeriodicalId":100387,"journal":{"name":"EcoEnergy","volume":"3 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ece2.95","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145129045","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
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EcoEnergy
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