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Boosting carrier utilization in Pr3+-doped long-afterglow photocatalysts through oxygen vacancy engineering for enhanced photo-Fenton degradation 通过氧空位工程提高Pr3+掺杂长余辉光催化剂的载流子利用率以增强光- fenton降解
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-01 Epub Date: 2025-03-29 DOI: 10.1016/j.jre.2025.03.033
Xiaoxuan Fan, Yonggui Zheng, Ran Tao, Lirong Xu, Shanshan Jiang, Hainan Li, Tianya Tan, Shuo Cao, Xuemei Lu, Kexin Wang, Jiwei Wang
Long-afterglow photocatalytic technology offers promising potential for all-weather pollutant treatment, yet its efficiency is often constrained by competition between afterglow emission and photocatalytic reactions. To address this, we developed a Pr3+-doped Ca2Al2SiO7 (CASO) photocatalyst enriched with oxygen vacancies (VO). The introduction of oxygen vacancies significantly increases trap concentration, enhancing both the intensity and duration of the afterglow emission. A persulfate-assisted photo-Fenton system was designed based on VO-CASO: Pr3+ enabling the self-activated degradation of tetracycline hydrochloride (TC) under ultraviolet afterglow. The photo-Fenton reaction consumes excess holes accumulated during the afterglow process, improving carrier utilization efficiency and mitigating rapid recombination. Additionally, persulfate addition can enrich reactive species and facilitate the Fe2+/Fe3+ cycle. Benefiting from these synergistic effects, VO-CASO: Pr3+ has achieved 75% TC degradation within 1 h, significantly outperforming traditional systems. This study provides a new strategy for enhancing long-afterglow photocatalytic performance, paving the way for sustainable pollutant degradation technologies.
长余辉光催化技术在全天候污染物处理中具有广阔的应用前景,但其效率往往受到余辉发射与光催化反应之间竞争的制约。为了解决这个问题,我们开发了一种富含氧空位(VO)的Pr3+掺杂Ca2Al2SiO7 (CASO)光催化剂。氧空位的引入显著提高了捕集阱的浓度,增强了余辉发射的强度和持续时间。设计了一种基于VO-CASO: Pr3+的过硫酸盐辅助光fenton系统,使其在紫外余辉下自激活降解盐酸四环素(TC)。光- fenton反应消耗了余光过程中积累的多余空穴,提高了载流子的利用效率,减轻了快速复合。此外,过硫酸盐的加入可以丰富反应物质,促进Fe2+/Fe3+的循环。得益于这些协同效应,VO-CASO: Pr3+在1小时内实现了75%的TC降解,显著优于传统系统。该研究为提高长余辉光催化性能提供了新的策略,为可持续污染物降解技术的发展铺平了道路。
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引用次数: 0
Electronic, magnetic, thermoelectric and optoelectronic properties of CaPr2(S/Se)4 for spintronic and energy applications 用于自旋电子和能量应用的CaPr2(S/Se)4的电子、磁、热电和光电子性质
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-01 Epub Date: 2025-04-11 DOI: 10.1016/j.jre.2025.04.002
Muhammad Rashid , A. Qadoos , Hanof Dawas Alkhaldi , Imed Boukhris , Q. Mahmood , Murefah Mana Al-Anazy , Zhenyi Jiang
This research presents a detailed ab initio density functional theory (DFT) analysis on magnetic, thermoelectric, and optoelectronic properties of CaPr2(S/Se)4 executed by Wien2k and Boltztrap2 packages for spintronic energy applications. The density of states, optimization energy, and negative formation energy all support the stability of the ferromagnetic state. The spin polarization density and Curie temperature (310 and 289 K) are also reported. In addition, the double exchange model, hybridization, density of states, band structures, exchange constants, exchange energies, and crystal field energies are addressed to ensure ferromagnetism by the spin of electrons. The magnetic moment of Pr shifts to Ca and S/Se sites, revealing that ferromagnetism is due to electron spin, not clustering of Pr magnetic ions. Thermoelectrics were evaluated by electrical conductivity (σ), thermal conductivity (ke), Seebeck coefficient (S), power factor (S2), and figures of merit (ZT). The room temperature values of S (0.169, 0.183 mV/K) and ZT (0.76, 0.90) increase their thermoelectric performance. Furthermore, dielectric function, refractive index, absorption coefficient α(ω), reflectivity R(ω), and other parameters are demonstrated in detail. Therefore, researchers can develop materials with the potential for spintronic and energy harvesting.
本研究利用Wien2k和Boltztrap2封装对CaPr2(S/Se)4的磁、热电和光电子性质进行了详细的从头算密度泛函理论(DFT)分析。态密度、优化能和负形成能都支持铁磁态的稳定性。报道了自旋极化密度和居里温度(310和289 K)。此外,还讨论了双交换模型、杂化、态密度、能带结构、交换常数、交换能和晶体场能,以确保电子自旋具有铁磁性。Pr的磁矩转移到Ca和S/Se位点,表明铁磁性是由于电子自旋,而不是Pr磁性离子的聚集。用电导率(σ)、导热系数(ke)、塞贝克系数(S)、功率因数(S2)和品质因数(ZT)对热电材料进行评价。室温S值(0.169,0.183 mV/K)和ZT值(0.76,0.90)提高了材料的热电性能。此外,还详细说明了介质函数、折射率、吸收系数α(ω)、反射率R(ω)等参数。因此,研究人员可以开发具有自旋电子和能量收集潜力的材料。
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引用次数: 0
Microstructure optimization and magnetic properties of sintered Nd-Fe-B via modulation of boron and gallium contents 硼和镓含量对烧结Nd-Fe-B的微观结构和磁性能的影响
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-01 Epub Date: 2025-02-18 DOI: 10.1016/j.jre.2025.02.006
Jingyan Zuo , Minggang Zhu , Dongmin Zhang , Ziqi Deng , Qisong Sun , Yaping Wu , Xiaolong Song , Xian Wu , Yikun Fang
The optimization of microstructure represents a significant methodology for enhancing coercivity (Hcj). This paper concentrates on optimizing the microstructure of magnets through the manipulation of the composition of low-melting-point and high-melting-point elements, thereby achieving the objective of augmenting the comprehensive magnetic properties of magnets. The present study is concerned with the microstructure of magnets comprising three distinct Ga and B contents, and the associated changes in their magnetic properties. The findings indicate that when the Ga content is 0.5 wt% and the B content is 0.88 wt%, the coercivity of the magnets is markedly enhanced. This is evidenced by an increase in coercivity from 8.51 to 14.83 kOe, representing a 74.26% rise. Concurrently, the residual magnetization strength of the magnet remains unaltered. This finding provides a crucial foundation for optimizing the overall magnetic properties of the magnets. The microstructural analysis indicates that a reduction in B content coupled with an increase in Ga content leads to the melting of sharp angles on the surface of the main-phase grains, facilitated by low-melting-point rare-earth-rich phases. This process results in the migration of Fe from the grain boundaries (GBs) to the triple junction phases (TJPs), while Nd migrates from the TJPs to the GBs. This migration results in a reduction in the agglomeration of rare-earth-rich elements within the TJPs, thereby increasing the Nd content in the GBs. This increase enhances the wettability of the GBs, while the reduction of Fe content in this phase mitigates the exchange-coupling effect between the main-phase GBs. Consequently, the GBs become more smooth, more homogeneous and more continuous, which ultimately results in an enhancement of the coercivity of the magnets.
微观结构的优化是提高矫顽力的重要方法。本文主要通过控制低熔点和高熔点元素的组成来优化磁体的微观结构,从而达到提高磁体综合磁性能的目的。本文研究了含有三种不同Ga和B含量的磁体的微观结构及其磁性能的相关变化。结果表明,当Ga含量为0.5 wt%, B含量为0.88 wt%时,磁体的矫顽力明显增强。矫顽力从8.51 k增加到14.83 k,增加了74.26%。同时,磁体的剩余磁化强度保持不变。这一发现为优化磁体的整体磁性提供了重要的基础。显微组织分析表明,B含量的降低和Ga含量的增加导致主相晶粒表面锐角的熔化,并由低熔点富稀土相促进。这一过程导致Fe从晶界(GBs)向三结相(TJPs)迁移,Nd从TJPs向GBs迁移。这种迁移导致富稀土元素在TJPs内的团聚减少,从而增加了GBs中的Nd含量。这种增加增强了GBs的润湿性,而该相中Fe含量的降低则减轻了主相GBs之间的交换耦合效应。因此,GBs变得更光滑,更均匀,更连续,这最终导致磁体的矫顽力增强。
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引用次数: 0
Defect engineering of ceria-based materials toward efficient electrocatalysis reaction 面向高效电催化反应的铈基材料缺陷工程
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-02-01 Epub Date: 2025-12-03 DOI: 10.1016/j.jre.2025.12.006
Botao Liu, Guiyao Dai, Shujun Hou, Huanli Wang, Dianxing Lian, Mohaoyang Chen, Chenxi Li, Weiwei Zhang, Ke Wu, Liwen Xing, Yongjun Ji
Cerium oxide (CeO2) with outstanding physiochemical properties, including special redox property, numerous oxygen vacancies, and high oxygen storage capacity (OSC), has attracted extensive research interests over the past few decades for electrocatalysis applications. This widespread applicability mainly originates from the ease in forming and repairing oxygen vacancies on the surface of ceria. Herein, this review provides a comprehensive overview of emerging progress related to defects modification of ceria-based nanomaterials, encompassing the fundamental characteristics of oxygen vacancy in ceria, advanced characterization methods and emerging theoretical approaches for understanding the properties of defects and predicting their effect on electrocatalytic behavior. To demonstrate the significance of defect-derived effects, electrochemical applications linked to defect engineering in ceria-based catalysts are explored. Finally, several probable challenges and future research directions concerning the defects controlling are discussed. We hope that the present review will provide an improved understanding of the roles of defects in determining the electrocatalytic performance of ceria-based materials.
氧化铈(CeO2)具有特殊的氧化还原性能、大量的氧空位和高氧存储容量(OSC)等优异的理化性质,在过去几十年里在电催化方面的应用引起了广泛的研究兴趣。这种广泛的适用性主要源于氧化铈表面的氧空位易于形成和修复。本文综述了铈基纳米材料缺陷改性的最新进展,包括氧化铈中氧空位的基本特征、先进的表征方法以及用于理解缺陷性质和预测其对电催化行为影响的新兴理论方法。为了证明缺陷衍生效应的重要性,研究了与缺陷工程相关的电化学应用在铈基催化剂中的应用。最后,对缺陷控制可能面临的挑战和未来的研究方向进行了讨论。我们希望本综述将提供一个更好的理解在确定铈基材料的电催化性能缺陷的作用。
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引用次数: 0
Boosting water oxidation activity of LaCoO3 by tailoring La3+ deficiency 通过调整La3+缺乏症提高LaCoO3的水氧化活性
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-02-01 Epub Date: 2025-05-28 DOI: 10.1016/j.jre.2025.05.016
Dipti Bhatt, Ravi K. Kunchala, Boddu S. Naidu
Developing an effective water oxidation catalyst is the key to achieving effective artificial photosynthesis. Using the sol–gel citrate approach, the metal oxide perovskite LaCoO3 was synthesized. Surface engineering of this perovskite material with acetic acid treatment boosts water oxidation. Acetic acid concentration was systematically varied from 0.1 to 5 mol/L to treat the LaCoO3 (LCO) for a fixed time. It is observed that among the tested samples, LaCoO3 treated with 1 mol/L acetic acid (LCO-1M) exhibits the highest water oxidation activity. The overpotential and Tafel slope are reduced from 603 to 500 mV and 217 to 155 mV/dec, respectively. LCO-1M shows 4.2 and 3.3 times higher turnover frequency than the pristine LCO for photochemical and electrochemical water oxidation, respectively. A boost in water-oxidation activity of these perovskites upon acid treatment is due to a decrease in the charge transfer resistance as well as contact angle brought about by the presence of mixed valence metal ions and enhanced oxygen vacancies on the surface, respectively. This method is beneficial to designing efficient catalysts for water oxidation.
开发有效的水氧化催化剂是实现有效人工光合作用的关键。采用溶胶-凝胶柠檬酸法合成了金属氧化物钙钛矿LaCoO3。该钙钛矿材料经醋酸处理后的表面工程促进了水的氧化。乙酸浓度在0.1 ~ 5 mol/L范围内变化,对LaCoO3 (LCO)进行固定时间的处理。结果表明,经1 mol/L乙酸(LCO-1M)处理的LaCoO3水氧化活性最高。过电位和Tafel斜率分别从603降低到500 mV和217降低到155 mV/dec。在光化学和电化学水氧化中,LCO- 1m的周转率分别是原始LCO的4.2倍和3.3倍。这些钙钛矿在酸处理后水氧化活性的提高是由于电荷转移电阻的降低以及表面上混合价金属离子的存在和氧空位的增强所带来的接触角的降低。该方法有助于设计高效的水氧化催化剂。
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引用次数: 0
Efficient electrocatalytic oxygen evolution enabled by porous Eu-Ni(PO3)2 nanosheet arrays 多孔Eu-Ni(PO3)2纳米片阵列实现高效电催化析氧
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-02-01 Epub Date: 2024-11-01 DOI: 10.1016/j.jre.2024.11.001
Pu Wang , Xiangrui Wu , Meng Li , Xuan Wang , Huiyu Wang , Qiuzi Huang , Hao Li , Yawen Tang , Gengtao Fu
Phosphorous compounds have garnered significant interest as catalysts for the oxygen evolution reaction (OER). However, their catalytic performance often falls short, limiting their widespread application in electrocatalysis. The objective of this work is to improve the OER performance of nickel metaphosphate (Ni(PO3)2) by incorporating rare-earth europium (Eu). The prepared Eu-Ni(PO3)2 exhibits significant electron redistribution and features porous nanosheet arrays. The optimized Eu-Ni(PO3)2 exhibits outstanding OER activity, with an overpotential of 273 mV at 10 mA/cm, rapid OER kinetics with a Tafel slope of 39.4 mV/dec, and excellent electrochemical stability. These results surpass the performance of Ni(PO3)2, many reported Ni-based catalysts, and even commercial RuO2. Operando Raman spectroscopy reveals that the improvement of OER performance on Eu-Ni(PO3)2 is due to the accelerated formation of surface NiOOH active species and the enhanced interfacial water enrichment during OER. Density functional theory (DFT) calculations further demonstrate that Eu doping induces electronic modulation between the Eu sites and adjacent O-Ni sites, resulting in an optimized thermodynamic pathway with balanced adsorption energies for key oxygen intermediates, thus alleviating thermodynamic limitations during OER.
磷化合物作为析氧反应(OER)的催化剂引起了人们极大的兴趣。然而,它们的催化性能往往不足,限制了它们在电催化中的广泛应用。本研究的目的是通过加入稀土铕(Eu)来改善偏磷酸镍(Ni(PO3)2)的OER性能。制备的Eu-Ni(PO3)2具有明显的电子重分布和多孔纳米片阵列。优化后的Eu-Ni(PO3)2表现出优异的OER活性,在10 mA/cm下的过电位为273 mV, OER动力学快速,Tafel斜率为39.4 mV/dec,电化学稳定性良好。这些结果超过了Ni(PO3)2,许多报道的Ni基催化剂,甚至是商业RuO2的性能。Operando拉曼光谱分析表明,eui - ni (PO3)2表面OER性能的提高是由于OER过程中表面NiOOH活性物质的加速形成和界面水富集的增强。密度泛函理论(DFT)计算进一步表明,Eu掺杂诱导了Eu位点和相邻O-Ni位点之间的电子调制,从而优化了关键氧中间体吸附能平衡的热力学途径,从而减轻了OER过程中的热力学限制。
{"title":"Efficient electrocatalytic oxygen evolution enabled by porous Eu-Ni(PO3)2 nanosheet arrays","authors":"Pu Wang ,&nbsp;Xiangrui Wu ,&nbsp;Meng Li ,&nbsp;Xuan Wang ,&nbsp;Huiyu Wang ,&nbsp;Qiuzi Huang ,&nbsp;Hao Li ,&nbsp;Yawen Tang ,&nbsp;Gengtao Fu","doi":"10.1016/j.jre.2024.11.001","DOIUrl":"10.1016/j.jre.2024.11.001","url":null,"abstract":"<div><div><span><span>Phosphorous compounds have garnered significant interest as catalysts for the oxygen evolution reaction (OER). However, their catalytic performance often falls short, limiting their widespread application in </span>electrocatalysis. The objective of this work is to improve the OER performance of nickel metaphosphate (Ni(PO</span><sub>3</sub>)<sub>2</sub><span>) by incorporating rare-earth europium (Eu). The prepared Eu-Ni(PO</span><sub>3</sub>)<sub>2</sub><span> exhibits significant electron redistribution and features porous nanosheet arrays. The optimized Eu-Ni(PO</span><sub>3</sub>)<sub>2</sub> exhibits outstanding OER activity, with an overpotential of 273 mV at 10 mA/cm, rapid OER kinetics with a Tafel slope of 39.4 mV/dec, and excellent electrochemical stability. These results surpass the performance of Ni(PO<sub>3</sub>)<sub>2</sub>, many reported Ni-based catalysts, and even commercial RuO<sub>2</sub>. <span><em>Operando</em></span><span> Raman spectroscopy reveals that the improvement of OER performance on Eu-Ni(PO</span><sub>3</sub>)<sub>2</sub><span> is due to the accelerated formation of surface NiOOH active species and the enhanced interfacial water enrichment during OER. Density functional theory (DFT) calculations further demonstrate that Eu doping induces electronic modulation between the Eu sites and adjacent O-Ni sites, resulting in an optimized thermodynamic pathway with balanced adsorption energies for key oxygen intermediates, thus alleviating thermodynamic limitations during OER.</span></div></div>","PeriodicalId":16940,"journal":{"name":"Journal of Rare Earths","volume":"44 2","pages":"Pages 595-603"},"PeriodicalIF":7.2,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146102715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Advanced rare earth oxide-based catalysts for thermal/electrocatalytic purification of gaseous pollutants 基于高级稀土氧化物的热/电催化净化气体污染物催化剂
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-02-01 Epub Date: 2025-11-27 DOI: 10.1016/j.jre.2025.11.017
Xiuxian Jiang , Tatsiana Shutava , Li Liu , Shuyan Song , Hongjie Zhang , Xiao Wang
Rare earth oxides, characterized by their distinctive physicochemical attributes, hold significant promise for the remediation of gaseous pollutants. A critical priority in advancing this field lies in the development of cost-effective catalytic systems. This review article provides a comprehensive overview of recent research progress in the rational design and fabrication of rare earth oxide-based catalysts, along with their implementation in strategies for gaseous pollutant abatement. Particular attention is given to the structure–performance correlations that underpin catalytic efficacy, as well as the elucidation of underlying reaction mechanisms. Furthermore, this work discusses the unresolved challenges hindering the practical deployment of rare earth oxide materials in real-world pollution control applications. Finally, forward-looking perspectives on emerging research directions are presented. This synthesis of current knowledge aims to serve as a valuable reference for researchers and engineers, offering both theoretical insights and practical guidance for the development of advanced rare earth oxide catalysts and their application in environmental remediation technologies.
稀土氧化物以其独特的物理化学特性为特征,在气体污染物的修复方面具有重要的前景。推进这一领域的一个关键优先事项是开发具有成本效益的催化系统。本文综述了近年来稀土氧化物基催化剂的合理设计和制备及其在气体污染物减排策略中的应用研究进展。特别注意的是结构-性能的相关性,支持催化效能,以及潜在的反应机制的阐明。此外,本工作讨论了阻碍稀土氧化物材料在实际污染控制应用中实际部署的未解决的挑战。最后,对新兴研究方向进行前瞻性展望。本文旨在为研究人员和工程师提供有价值的参考,为先进稀土氧化物催化剂的开发及其在环境修复技术中的应用提供理论见解和实践指导。
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引用次数: 0
Multifunctionality exploration of dysprosium-doped NiFe2O4: An efficient bifunctional electrocatalyst toward ORR/OER 镝掺杂NiFe2O4的多功能探索:一种高效的ORR/OER双功能电催化剂
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-02-01 Epub Date: 2025-03-25 DOI: 10.1016/j.jre.2025.03.023
A.R. Panda , S. Samanta , S. Banerjee , P. Parhi
Electrocatalysts are essential for accelerating the kinetics of oxygen evolution reaction (OER) and oxygen reduction reactions (ORR) in various air-based energy conversion and storage systems, including fuel cells and metal-air batteries. The hunt for more affordable catalysts has been sparked by the limited natural availability and high cost of noble metals used in both ORR and OER. Inexpensive metal oxides are good alternatives as they have demonstrated a comparable level of activity (as compared to noble metal-based systems) for a variety of electrochemical processes. The present study reveals a facile strategy to prepare rare earth-doped transition metal ferrite spinel (NiDyxFe2–xO4) as an efficient bifunctional catalyst. NiDyxFe2–xO4 with B-site doping of dysprosium (x = 0.025, 0.05, 0.075, 0.1) was prepared by sol–gel method. The prepared catalysts were characterized using different characterization techniques such as X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), ultraviolet–visible spectroscopy (UV–Vis), and Brunauer–Emmett–Teller (BET) method. The bifunctional catalytic behavior of the prepared catalyst towards both ORR and OER was studied in an alkaline medium. The catalysts denoted as NDFO-0.025, NDFO-0.05, NDFO-0.075, and NDFO-0.1 respectively for different doping Dy (x = 0.025, 0.05, 0.075, 0.1) show improved kinetics and activity for both ORR and OER. Among the prepared electrocatalysts NDFO-0.05 shows bifunctional behavior having an onset potential of 0.844 V vs. RHE and a current density of 5.6 mA/cm2. For OER, NDFO-0.05 exhibits an onset potential of 1.59 V (vs. RHE) and a current density of 36 mA/cm2, a high electron transfer number n nearly equal to 4 and long-term stability better than that of commercial Pt/C.
在燃料电池和金属-空气电池等各种空气基能量转换和存储系统中,电催化剂对于加速析氧反应(OER)和氧还原反应(ORR)的动力学至关重要。由于ORR和OER中使用的贵金属天然可用性有限且成本高,因此人们开始寻找更经济实惠的催化剂。廉价的金属氧化物是很好的替代品,因为它们在各种电化学过程中表现出相当水平的活性(与贵金属基系统相比)。本研究揭示了一种制备稀土掺杂过渡金属铁素体尖晶石(NiDyxFe2-xO4)作为高效双功能催化剂的简单策略。采用溶胶-凝胶法制备了b位掺杂镝(x = 0.025, 0.05, 0.075, 0.1)的NiDyxFe2-xO4。采用x射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、扫描电子显微镜(SEM)、x射线光电子能谱(XPS)、透射电子显微镜(TEM)、紫外可见光谱(UV-Vis)和布鲁诺尔-埃米特-泰勒(BET)等表征技术对所制备的催化剂进行了表征。在碱性介质中研究了所制备的催化剂对ORR和OER的双功能催化行为。不同掺杂Dy (x = 0.025, 0.05, 0.075, 0.1)的NDFO-0.025、NDFO-0.05、NDFO-0.075和NDFO-0.1催化剂的ORR和OER动力学和活性均有所提高。在所制备的电催化剂中,NDFO-0.05表现出双功能行为,相对于RHE的起始电位为0.844 V,电流密度为5.6 mA/cm2。对于OER, NDFO-0.05的起始电位为1.59 V(相对于RHE),电流密度为36 mA/cm2,电子转移数n接近4,长期稳定性优于商用Pt/C。
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引用次数: 0
Rare-earth modification optimizes porous Fe-N-C catalysts to boost oxygen reduction reaction for Zn-air batteries 稀土改性优化多孔Fe-N-C催化剂,促进锌空气电池的氧还原反应
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-02-01 Epub Date: 2025-03-18 DOI: 10.1016/j.jre.2025.03.015
Jiao Yang , Jiayi Cui , Yujuan Zhuang , Jianmin Yu , Lishan Peng
Fe-N-C electrocatalysts have garnered significant interest for their effectiveness in the oxygen reduction reaction. However, optimizing the local coordination of Fe sites and achieving a high density of accessible active sites continue to present considerable challenges. In this work, we introduced lanthanum (La) into the Fe-N-C catalyst via a multi-step process combining ion adsorption and pyrolysis, resulting in a La-modified, porous Fe-N-C catalyst (FeLaDA-NC). The incorporation of La enhances the intrinsic catalytic properties of Fe centers, while the optimized synthesis method increases the density of available FeNx active sites. The FeLaDA-NC catalyst exhibits remarkable ORR activity, with a half-wave potential of 0.88 V, alongside excellent stability and methanol tolerance, outperforming commercial Pt/C catalysts. When using the FeLaDA-NC as ORR catalyst, the zinc-air battery demonstrates an impressive peak power density of 173.2 mW/cm2, highlighting the advantages of tailoring the coordination of Fe-N-C catalysts. This study highlights the promising potential of rare-earth modification in advancing the catalytic performance of Fe-based electrocatalysts.
Fe-N-C电催化剂因其在氧还原反应中的有效性而引起了人们的极大兴趣。然而,优化铁位点的局部协调和实现可达活性位点的高密度仍然是相当大的挑战。在这项工作中,我们通过离子吸附和热解相结合的多步骤工艺将镧(La)引入到Fe-N-C催化剂中,得到了La改性的多孔Fe-N-C催化剂(FeLaDA-NC)。La的加入增强了Fe中心的内在催化性能,而优化后的合成方法增加了有效的FeNx活性位点的密度。FeLaDA-NC催化剂表现出显著的ORR活性,半波电位为0.88 V,具有优异的稳定性和甲醇耐受性,优于商用Pt/C催化剂。当使用FeLaDA-NC作为ORR催化剂时,锌-空气电池显示出令人印象深刻的峰值功率密度为173.2 mW/cm2,突出了Fe-N-C催化剂定制配位的优势。本研究强调了稀土改性在提高铁基电催化剂催化性能方面的巨大潜力。
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引用次数: 0
Structural engineering of metal–organic frameworks for enhanced electrocatalytic urea oxidation reaction: Mechanistic insights and electronic modulation strategies 增强电催化尿素氧化反应的金属-有机框架的结构工程:机理见解和电子调制策略
IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-02-01 Epub Date: 2025-08-27 DOI: 10.1016/j.jre.2025.08.016
Bin Hu , Kun Chen , Bingbing Shen , Xiaohong Shang , Fenghe Duan , Chuanpan Guo , Shuai Zhang , Zhihong Zhang
Electrocatalytic urea oxidation reaction (UOR) not only provides innovative solutions for clean energy development and environmental pollution control, but also promotes sustainable development through efficient resource recycling. Its technological breakthroughs hold significant implications for achieving carbon neutrality goals and establishing a green energy system. Benefiting from their high specific surface area, tunable pore structures, and modifiable electronic properties, diverse metal–organic frameworks (MOFs)-based UOR electrocatalysts have been exploited, such as pristine Ni-, Fe-, and Cu-based monometallic, bimetallic, or multiple metallic MOFs, MOFs-based composites, and MOFs-related derivatives. The porous framework exposes abundant active sites and enhances mass transfer, while the synergy between metal nodes and organic ligands optimizes electronic configurations to reduce reaction energy barriers. By integrating conductive substrates or constructing heterostructures, catalytic activity and stability are significantly enhanced. Varieties of strategies have been performed to further decrease the overpotential and accelerate the kinetics towards the UOR, such as modulating charge density and d-band center positions of active sites through metal–ligand coordination, inducing charge redistribution and enhancing electron transport via heterostructure interfaces, breaking electronic symmetry and boosting surface reactivity through defect engineering, adjusting atomic spacing and electronic band structures via strain engineering, reinforcing charge transfer and stabilizing active sites using conductive substrates, and enabling precise design through dynamic in-situ reconstruction and theory-guided optimization. This review explores the latest significant advances in the design and synthesis of MOFs-based UOR catalysts. Beyond highlighting recent breakthroughs in UOR catalysts, this review critically emphasizes the design strategies for urea electrolysis in the field of energy conversion and systematically addresses current challenges. Furthermore, this comprehensive research approach proposes forward-looking strategies for future research directions in energy conversion and carbon neutrality to advance the development of this emerging field.
电催化尿素氧化反应(UOR)不仅为清洁能源开发和环境污染控制提供了创新的解决方案,而且通过高效的资源循环利用促进了可持续发展。其技术突破对实现碳中和目标和建立绿色能源体系具有重要意义。得益于其高比表面积、可调节的孔结构和可改变的电子性能,各种金属有机骨架(MOFs)基UOR电催化剂已经被开发出来,例如原始的Ni、Fe和cu基单金属、双金属或多金属MOFs、MOFs基复合材料以及MOFs相关衍生物。多孔框架暴露了丰富的活性位点,增强了传质,而金属节点和有机配体之间的协同作用优化了电子构型,降低了反应能垒。通过整合导电底物或构建异质结构,催化活性和稳定性显著提高。为了进一步降低过电位,加速向UOR方向发展的动力学,研究人员采用了多种策略,如通过金属配位调节活性位点的电荷密度和d带中心位置,通过异质结构界面诱导电荷再分配和增强电子传递,通过缺陷工程打破电子对称性和提高表面反应性。通过应变工程调整原子间距和电子能带结构,利用导电衬底加强电荷转移和稳定活性位点,并通过动态原位重构和理论指导优化实现精确设计。本文综述了基于mofs的UOR催化剂的设计和合成的最新重大进展。除了强调UOR催化剂的最新突破外,本文还重点介绍了尿素电解在能量转换领域的设计策略,并系统地解决了当前的挑战。此外,该综合研究方法为能源转换与碳中和的未来研究方向提出了前瞻性策略,以推动这一新兴领域的发展。
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Journal of Rare Earths
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