Journal of Rare Earths最新文献_第2页

Construction of triple interfaces to tailor electronic structure and local microenvironment of ruthenium species in Rusp/TiO2–x-CeO2–x for enhanced hydrogen energy conversion 在Rusp/ TiO2-x-CeO2-x中构建三重界面以调整钌的电子结构和局部微环境以增强氢能转换

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.10.018

Yuanyuan Cong , Yu Gao , Xiaobo Zheng , Huibin Lai , Qiuping Zhao , Chunlei Li , Yilong Zhang , Mengling Liu

The rational design of heterostructures to simultaneously optimize local environments and electronic configurations in electrocatalysts represents a promising strategy for enhancing hydrogen oxidation (HOR) and evolution (HER) reactions, crucial for advancing next-generation anion exchange membrane fuel cells and water electrolyzers. Herein, we report a novel Ru_sp/TiO_2–x-CeO_2–x electrocatalyst with a triple-interface structure, where Ru species are anchored on the surface of both TiO_2–x and CeO_2–x. This engineered Ru_sp/TiO_2–x-CeO_2–x exhibits exceptional hydrogen energy conversion in the alkaline solution, significantly outperforming Pt/C. Specifically, the HOR mass activity reaches up to 4978 A/g_Ru, which is 16 times that of Pt/C (310 A/g_Pt). Meanwhile, the HER overpotential at 10 mA/cm² is only 21 mV, 37 mV lower than that of Pt/C. More importantly, the Ru_sp/TiO_2–x-CeO_2–x demonstrates excellent anti-oxidation ability, maintaining activity even at potentials as high as 1.2 V vs. RHE. Through comprehensive characterization combining electrochemical results, density functional theory (DFT) calculations, in situ Raman spectroscopy, and in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), we elucidate the dual synergistic effects governing the superior performance: (i) the electron-rich Ru centers induced by TiO_2–x-CeO_2–x hybridization effectively weaken adsorption energetics of key intermediates (H_ad, OH_ad, CO_ad); and (ii) the unique metal-support interaction creates a local acid environment, which promotes the transport of intermediate species.

合理设计异质结构，同时优化电催化剂的局部环境和电子构型，是促进氢氧化（HOR）和进化（HER）反应的一种有前途的策略，对推进下一代阴离子交换膜燃料电池和水电解槽至关重要。本文报道了一种新型的Rusp/ TiO2-x - CeO2-x电催化剂，其具有三界面结构，其中Ru物质被锚定在TiO2-x和CeO2-x表面。这种设计的Rusp/ TiO2-x-CeO2-x在碱性溶液中表现出优异的氢能转换，显著优于Pt/C。其中，HOR质量活度高达4978 A/gRu，是Pt/C （310 A/gPt）的16倍。同时，在10 mA/cm2时，HER过电位仅为21 mV，比Pt/C低37 mV。更重要的是，Rusp/ TiO2-x-CeO2-x表现出优异的抗氧化能力，即使在高达1.2 V的电位下也能保持活性。通过结合电化学结果、密度泛函数理论（DFT）计算、原位拉曼光谱和原位衰减全反射表面增强红外吸收光谱（ATR-SEIRAS）的综合表征，我们阐明了控制优异性能的双重协同效应：(i) TiO2-x-CeO2-x杂化诱导的富电子Ru中心有效地削弱了关键中间体（Had, OHad, COad）的吸附能量；(2)独特的金属-载体相互作用创造了一个局部酸环境，促进了中间物种的运输。

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引用次数: 0

Enhancing electrocatalytic methanol oxidation using La-doped PtRhLa multimetallic catalysts la掺杂PtRhLa多金属催化剂增强电催化甲醇氧化

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.02.003

Chunmei Xiahou , Mingli Ouyang , Lihua Zhu , An Pei , Yingliang Feng , Tongxiang Liang

The development of noble metal catalysts with sustained high activity is essential for advancing direct alcohol fuel cells (DAFCs). In this work, we synthesized various catalysts containing Pt, Rh, and La, supported on carbon black, via a simple liquid phase chemical reduction method, enhancing their resistance to CO poisoning and promoting electrocatalytic methanol oxidation reaction (MOR). The PtRhLa/C catalyst demonstrates a low CO₂ generation onset potential and exceptional MOR activity, achieving a mass activity of 2.83 A/mgₚₜ, which is 7 times greater than that of 20 wt% Pt/C (Pt/C-JM) (0.40 A/mgₚₜ). The catalysts were characterized and tested by X-ray diffraction (XRD), X-ray spectroscopy (XPS), scanning transmission electron microscopy (STEM) and in-situ Fourier transform infrared (FTIR) reflection spectroscopy. The results confirm that the incorporation of the oxygenophilic element Rh and rare earth element La effectively fine-tunes the coordination environment and electronic structure of Pt, weakening the Pt–CO bond and enhancing conductivity, MOR performance, and stability. This study highlights the potential of oxygenophilic and rare earth element-doped materials for electrocatalytic MOR and provides valuable insights for the future development of DAFCs.

开发具有持续高活性的贵金属催化剂是推进直接醇燃料电池（DAFCs）发展的关键。本研究通过简单的液相化学还原法合成了以炭黑为载体的Pt、Rh、La等多种催化剂，增强了其抗CO中毒能力，促进了电催化甲醇氧化反应（MOR）的发生。PtRhLa/C催化剂具有较低的CO₂生成起始电位和优异的MOR活性，其质量活性为2.83 a/ mgₚµl，是20% wt% Pt/C (Pt/C- jm) （0.40 a/ mgₚµl）的7倍。采用x射线衍射（XRD）、x射线能谱（XPS）、扫描透射电子显微镜（STEM）和原位傅里叶变换红外（FTIR）反射光谱对催化剂进行了表征和测试。结果证实，亲氧元素Rh和稀土元素La的掺入有效地微调了Pt的配位环境和电子结构，减弱了Pt - co键，提高了导电性能、MOR性能和稳定性。该研究强调了亲氧材料和稀土元素掺杂材料在电催化MOR中的潜力，并为DAFCs的未来发展提供了有价值的见解。

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引用次数: 0

Advances in rare earth catalysts for small molecule electrosynthesis 稀土小分子电合成催化剂研究进展

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.02.009

Junfeng Du , Jing Yu , Chaohui Guan, Tao Chen, Fei Yao, Shuai Zhang, Haibin Chu

Electrosynthesis leverages electrochemical reactions to transform simple molecules into complex compounds using renewable, clean energy from sources like wind and solar power. This technology has shown promise for economically converting excess atmospheric carbon dioxide and nitrogen oxides into value-added products through electrochemical reduction. Additionally, the oxidation of biomass-derived substrates, such as 5-hydroxymethylfurfural (HMF) and glycerol, can serve as alternative anodic reactions to the oxygen evolution reaction (OER), which typically requires a higher voltage and yields lower-value products. This substitution improves the overall economic efficiency of electrosynthesis processes. Notably, the unique 4f electronic structure of rare earth elements not only increases the number of active sites and stabilizes these catalysts, but also modulates the adsorption of reaction intermediates on electrocatalysts, thereby enhancing the product selectivity. As a result, rare earth elements have found broad applications across diverse electrosynthesis reactions.

电合成利用电化学反应，利用风能和太阳能等可再生清洁能源，将简单分子转化为复杂化合物。这项技术有望通过电化学还原将大气中过量的二氧化碳和氮氧化物经济地转化为增值产品。此外，生物质衍生底物的氧化，如5-羟甲基糠醛（HMF）和甘油，可以作为析氧反应（OER）的替代阳极反应，后者通常需要更高的电压，产生更低价值的产物。这种替代提高了电合成过程的整体经济效率。值得注意的是，稀土元素独特的4f电子结构不仅增加了活性位点的数量，稳定了这些催化剂，而且调节了反应中间体在电催化剂上的吸附，从而提高了产物的选择性。因此，稀土元素在不同的电合成反应中得到了广泛的应用。

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引用次数: 0

Carbon in situ supported Ni/CeO2 heterogeneous catalyst with rich interfaces for efficient electrocatalysis 具有丰富界面的原位负载Ni/CeO2非均相催化剂

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.02.005

Xiaodan Yang , Yuan Zhang , Shimin Zhang , Hongming Sun , Xiang Chen , Chengpeng Li

Constructing strong-coupling and high-density interfaces is crucial for achieving high performance of metal/oxide heterogeneous catalysts, yet remains a significant challenge. Here, we developed a carbon auxiliary “microreactor” method to prepare the metal/oxide composites with rich heterogeneous interfaces and strong electronic metal-oxide interaction. Employing this innovative strategy, we synthesized a Ni/CeO₂ heterogeneous catalyst that is in situ loaded onto carbon substrate (Ni/CeO₂@C), which shows excellent performance for hydrogen evolution reaction (HER) in alkaline media. Specifically, the Ni/CeO₂@C catalyst displays a low overpotential (75 mV) to drive a current density of 10 mA/cm² with a low Tafel slope (65.1 mV/dec). The rich interfaces between Ni and CeO₂ offer abundant dual active sites that accelerate the dissociation of water (Volmer step) and optimize the hydrogen adsorption energy (Heyrovsky step). This synergy significantly improves the overall kinetics of the HER. This method is universal and offers great potential for preparing carbon in situ supported heterogeneous nanomaterials with rich interfaces, enabling the high performance for electrocatalysis.

构建强耦合和高密度界面是实现金属/氧化物非均相催化剂高性能的关键，但仍然是一个重大挑战。在此，我们开发了一种碳辅助“微反应器”方法来制备具有丰富非均相界面和强电子金属-氧化物相互作用的金属/氧化物复合材料。利用这一创新策略，我们合成了原位负载于碳基（Ni/CeO2@C）上的Ni/CeO2非均相催化剂，该催化剂在碱性介质中表现出优异的析氢反应（HER）性能。具体来说，Ni/CeO2@C催化剂显示出低过电位（75 mV），可以驱动10 mA/cm2的电流密度和低塔菲尔斜率（65.1 mV/dec）。Ni和CeO2之间丰富的界面提供了丰富的双活性位点，加速了水的解离（Volmer步骤），优化了氢的吸附能（Heyrovsky步骤）。这种协同作用显著改善了HER的整体动力学。该方法具有通用性，为制备具有丰富界面的碳原位负载非均相纳米材料提供了巨大的潜力，使其具有高性能的电催化性能。

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引用次数: 0

Synthesis and characterization of Ce-MOF-based flexible electrode materials for uric acid sensing and oxygen evolution reaction ce - mof基尿酸传感及出氧反应柔性电极材料的合成与表征

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.06.008

Huanxi Zhang , Jianhui Liu , Chunhuan Xu , Sijia Zhang , Xuechuan Gao

Electrochemical biosensors and the oxygen evolution reaction (OER) represent two pivotal directions in the field of electrochemistry. In this study, a bifunctional integrated flexible electrode material (Ce-MOF-CNT-COOH_x/PVA_y) was developed, capable of both uric acid recognition and water electrolysis for oxygen evolution. The synthesis process began with the modification of Ce-MOFs by incorporating carboxylated carbon nanotubes (CNT-COOH), resulting in Ce-MOF-CNT-COOH_x with varying degrees of CNT-COOH doping. Subsequently, Ce-MOF-CNT-COOH_x was compounded with polyvinyl alcohol (PVA) films of different thicknesses to produce Ce-MOF-CNT-COOH_x/PVA_y composites. Through cyclic voltammetry (CV) and linear sweep voltammetry (LSV) analyses, the Ce-MOF-CNT-COOH₂₀/PVA_1.2 composite emerges as the top performer. Following its identification as the optimal material, the Ce-MOF-CNT-COOH₂₀/PVA_1.2 composite was evaluated for uric acid recognition in a phosphate buffer solution at pH 7.4. The results demonstrate rapid uric acid detection (less than 5 s), with a sensitivity of 45.69 μA·L/(mmol·cm²). The linear detection range is found to be 1–9 mmol/L, and the detection limit is determined to be 69.53 μmol/L. Furthermore, Ce-MOF-CNT-COOH₂₀/PVA_1.2 exhibits exceptional specificity and remarkable cyclic stability. In addition to its biosensing capabilities, the OER performance of Ce-MO-CNT-COOH₂₀/PVA_1.2 material was assessed. At a current density of 10 mA/cm², the overpotential was measured at 321 mV, outperforming the benchmark water electrolysis catalyst IrO₂ (357 mV). The Ce-MOF-CNT-COOH₂₀/PVA_1.2 material also displays lower resistance and superior durability, further highlighting its potential for practical applications. The application of this proposed Ce-MOF-CNT-COOH₂₀/PVA_1.2 bifunctional flexible electrode material demonstrates the significant potential of rare-earth MOF-based materials in both electrochemical sensing and electrocatalysis.

电化学生物传感器和析氧反应（OER）是电化学领域的两个关键方向。在这项研究中，开发了一种双功能集成柔性电极材料（Ce-MOF-CNT-COOHx/PVAy），既能识别尿酸，又能电解水析氧。合成过程从加入羧化碳纳米管（CNT-COOH）对ce - mof进行改性开始，得到不同程度掺杂CNT-COOH的Ce-MOF-CNT-COOHx。随后，将Ce-MOF-CNT-COOHx与不同厚度的聚乙烯醇（PVA）膜复配，制备Ce-MOF-CNT-COOHx/PVAy复合材料。通过循环伏安法（CV）和线性扫描伏安法（LSV）分析，Ce-MOF-CNT-COOH20/PVA1.2复合材料表现最佳。将Ce-MOF-CNT-COOH20/PVA1.2复合材料确定为最佳材料后，在pH为7.4的磷酸盐缓冲溶液中评估其尿酸识别能力。结果表明，该方法可快速检测尿酸（≤5 s），灵敏度为45.69 μA·L/（mmol·cm2）。线性检测范围为1 ~ 9 mmol/L，检出限为69.53 μmol/L。此外，Ce-MOF-CNT-COOH20/PVA1.2表现出卓越的特异性和显著的循环稳定性。除了生物传感能力外，还评估了Ce-MO-CNT-COOH20/PVA1.2材料的OER性能。在电流密度为10 mA/cm2时，过电位为321 mV，优于基准电解水催化剂IrO2 （357 mV）。Ce-MOF-CNT-COOH20/PVA1.2材料还显示出较低的电阻和优异的耐久性，进一步突出了其实际应用潜力。本文提出的Ce-MOF-CNT-COOH20/PVA1.2双功能柔性电极材料的应用证明了稀土mof基材料在电化学传感和电催化方面的巨大潜力。

{"title":"Synthesis and characterization of Ce-MOF-based flexible electrode materials for uric acid sensing and oxygen evolution reaction","authors":"Huanxi Zhang , Jianhui Liu , Chunhuan Xu , Sijia Zhang , Xuechuan Gao","doi":"10.1016/j.jre.2025.06.008","DOIUrl":"10.1016/j.jre.2025.06.008","url":null,"abstract":"<div><div>Electrochemical biosensors and the oxygen evolution reaction (OER) represent two pivotal directions in the field of electrochemistry. In this study, a bifunctional integrated flexible electrode material (Ce-MOF-CNT-COOHx/PVAy) was developed, capable of both uric acid recognition and water electrolysis for oxygen evolution. The synthesis process began with the modification of Ce-MOFs by incorporating carboxylated carbon nanotubes (CNT-COOH), resulting in Ce-MOF-CNT-COOHx with varying degrees of CNT-COOH doping. Subsequently, Ce-MOF-CNT-COOHx was compounded with polyvinyl alcohol (PVA) films of different thicknesses to produce Ce-MOF-CNT-COOHx/PVAy composites. Through cyclic voltammetry (CV) and linear sweep voltammetry (LSV) analyses, the Ce-MOF-CNT-COOH20/PVA1.2 composite emerges as the top performer. Following its identification as the optimal material, the Ce-MOF-CNT-COOH20/PVA1.2 composite was evaluated for uric acid recognition in a phosphate buffer solution at pH 7.4. The results demonstrate rapid uric acid detection (less than 5 s), with a sensitivity of 45.69 μA·L/(mmol·cm2). The linear detection range is found to be 1–9 mmol/L, and the detection limit is determined to be 69.53 μmol/L. Furthermore, Ce-MOF-CNT-COOH20/PVA1.2 exhibits exceptional specificity and remarkable cyclic stability. In addition to its biosensing capabilities, the OER performance of Ce-MO-CNT-COOH20/PVA1.2 material was assessed. At a current density of 10 mA/cm2, the overpotential was measured at 321 mV, outperforming the benchmark water electrolysis catalyst IrO2 (357 mV). The Ce-MOF-CNT-COOH20/PVA1.2 material also displays lower resistance and superior durability, further highlighting its potential for practical applications. The application of this proposed Ce-MOF-CNT-COOH20/PVA1.2 bifunctional flexible electrode material demonstrates the significant potential of rare-earth MOF-based materials in both electrochemical sensing and electrocatalysis.</div></div>","PeriodicalId":16940,"journal":{"name":"Journal of Rare Earths","volume":"44 2","pages":"Pages 616-629"},"PeriodicalIF":7.2,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146102716","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

CeO2/ZnO heterojunction as an efficient catalyst for electrocatalytic nitrogen reduction reaction via an “electron pump” effect CeO2/ZnO异质结通过电子泵效应作为电催化氮还原反应的高效催化剂

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.03.012

Jingxian Li , Jun Wang , Guixi Wang , Shulin Zhao , Zhiyu Yang , Xiaoxuan Wang , Yi-Ming Yan

The development of efficient catalysts for the electrocatalytic nitrogen reduction reaction (ENRR) is crucial for sustainable ammonia production. In this study, we report the synthesis and characterization of a CeO₂/ZnO heterojunction, demonstrating remarkable catalytic performance for ENRR. The heterostructure facilitates an “electron pump” effect, enhancing electron transfer and promoting nitrogen activation. The synthesized CeO₂/ZnO was characterized using scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), ultraviolet photoelectron spectroscopy (UPS), along with other analytical techniques. The material exhibits remarkable performance in ENRR, achieving an NH₃ yield of 60.21 μg/(h·mg_cat) at −0.2 V versus reversible hydrogen electrode (RHE) and a Faradaic efficiency of 11.48% at −0.2 V versus RHE with an aqueous 0.1 mol/L Li₂SO₄ electrolyte. The enhanced performance is attributed to the synergistic interaction between CeO₂ and ZnO, which optimizes the electronic structure and surface properties. This research elucidates the catalytic mechanisms through which CeO₂ enhances the ENRR activity of ZnO, offering novel insights into the application of rare earth elements.

开发高效的电催化氮还原反应（ENRR）催化剂是实现可持续氨生产的关键。在本研究中，我们报道了CeO2/ZnO异质结的合成和表征，该异质结对ENRR具有显著的催化性能。异质结构有利于“电子泵”效应，增强电子转移，促进氮活化。采用扫描电镜（SEM）、透射电镜（TEM）、x射线衍射（XRD）、x射线光电子能谱（XPS）、紫外光电子能谱（UPS）等分析技术对合成的CeO2/ZnO进行了表征。该材料在ENRR中表现出优异的性能，与可逆氢电极（RHE）相比，在−0.2 V时NH3产率为60.21 μg/(h·mgcat)，在0.1 mol/L Li2SO4水溶液下，Faradaic效率为11.48%。性能的增强是由于CeO2和ZnO之间的协同作用，优化了电子结构和表面性能。本研究阐明了CeO2增强ZnO ENRR活性的催化机制，为稀土元素的应用提供了新的见解。

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引用次数: 0

Water oxidation promoted synergistically by CeO2-shell on CoNiO2-core ceo2壳在cono2核上协同促进水氧化

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.08.011

Bolin Zhao , Rana Muhammad Irfan , Chuhao Liu , Shamraiz Hussain Talib , Azhar Mahmood , Li Niu

Rare-earth based transition metal oxides have proved to be the most promising candidates in the exploration of non-precious oxygen evolution reaction (OER) catalysts. However, the knowledge regarding their active sites and electrocatalytic mechanism is very limited due to their different crystallization behaviors and there are still big challenges in the efficient coupling of transition and rare-earth metals with full utilization of active sites. To improve and stabilize OER catalysis, we developed the core–shell CeO₂@CoNiO₂ nanoplates (NPLs) for enhanced and stable OER catalysis. Surprisingly, CeO₂ shell regulates the electronic structure of CoNiO₂ core and increases the number of active sites and oxygen vacancies to achieve high electrochemical performance in a three-electrode system. Compared with CoNiO₂ nanoparticles, the developed core–shell NPLs exhibit favorable performance with an overpotential of only 206 mV at 10 mA/cm² and robust electrochemical stability of 500 h at 10 mA/cm² and 300 h at 50 mA/cm². In situ Raman spectroscopy unveils that CeO₂@CoNiO₂ is structurally more stable than CoNiO₂, which is consistent with its performance persistence. Besides, theoretical calculations confirm that the Ce shell serves as the active centers for OER, and the formed core–shell metal oxides NPLs promote the adsorption and dissociation of water, thus causing the fast generation of O₂. This work provides a new perspective for designing highly active core–shell structure of mixed metal oxides of transition and rare-earth metals for OER.

稀土基过渡金属氧化物已被证明是探索非贵重析氧反应（OER）催化剂中最有前途的候选材料。然而，由于它们的结晶行为不同，对它们的活性位点和电催化机理的了解非常有限，在充分利用活性位点的情况下，如何有效地耦合过渡金属和稀土金属仍然存在很大的挑战。为了改善和稳定OER催化，我们开发了核壳纳米板CeO2@CoNiO2 （NPLs）来增强和稳定OER催化。令人惊讶的是，CeO2外壳调节了CoNiO2核心的电子结构，增加了活性位点和氧空位的数量，从而在三电极体系中实现了高电化学性能。与CoNiO2纳米粒子相比，所制备的核壳型NPLs表现出良好的性能，在10 mA/cm2下过电位仅为206 mV，在10 mA/cm2下电化学稳定性为500 h，在50 mA/cm2下电化学稳定性为300 h。原位拉曼光谱揭示了CeO2@CoNiO2在结构上比CoNiO2更稳定，这与其性能持久性是一致的。此外，理论计算证实Ce壳层是OER的活性中心，形成的核壳金属氧化物NPLs促进了水的吸附和解离，从而导致O2的快速生成。本研究为OER中过渡金属和稀土金属混合氧化物的高活性核壳结构设计提供了新的思路。

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引用次数: 0

Vacancy defect-rich NiS2 nanosheets induced by Ce-doping for highly efficient water and urea oxidation reaction ce掺杂诱导的富空位缺陷NiS2纳米片用于高效水尿素氧化反应

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.06.014

Biying Tian , Yaqin Chen , Jiawen Sun, Yi-Ru Hao, Chunhao Li, Jing Sun, Hui Xue, Qin Wang

The feasibility of enhancing the electrocatalytic performance of sulfides is demonstrated through element doping and vacancy engineering. However, the investigation on the reaction mechanisms of catalyst doping and defects related to oxygen evolution reaction (OER) still faces significant challenges. In this work, a Ce-doped NiS₂ supported on carbon cloth (Ce-NiS₂@CC) with abundant sulfur vacancy defects was successfully developed through a sequential two-step hydrothermal and high-temperature vulcanization strategy. The results demonstrate that the obtained Ce-NiS₂@CC catalyst exhibits excellent electrochemical performance for both OER and urea oxidation reaction (UOR). It requires only 1.40 and 1.28 V to achieve a current density of 10 mA/cm² for OER and UOR, respectively. Furthermore, the Tafel slopes observed for OER and UOR are noteworthy at 40.2 and 58.3 mV/dec, respectively, suggesting enhanced kinetics and superior catalytic performance. Additionally, the stability tests conducted on the catalyst reveal that the Ce-NiS₂@CC possesses exceptional electrochemical long-term stability, making it a highly reliable and durable option for various applications. Density functional theory calculations and in situ Raman results demonstrate that Ce doping and sulfur vacancy synergistically promote surface reconstruction to form Ni^Ⅲ–O species, modulate the local charge distribution near the Ni site, thereby facilitating the adsorption and activation of water molecules, and consequently accelerating the kinetics of OER. This study systematically investigated the impact of metal doping and vacancy defects on electrocatalytic performance, offering insights into electronic structure regulation and performance optimization for efficient electrocatalysts.

通过元素掺杂和空位工程论证了提高硫化物电催化性能的可行性。然而，对催化剂掺杂的反应机理和与析氧反应（OER）有关的缺陷的研究仍面临重大挑战。通过连续两步水热和高温硫化策略，成功地制备了一种富含硫空位缺陷的碳布（Ce-NiS2@CC）负载的ce掺杂NiS2。结果表明，Ce-NiS2@CC催化剂在OER和尿素氧化反应（UOR）中均表现出优异的电化学性能。OER和UOR分别只需要1.40和1.28 V就能实现10 mA/cm2的电流密度。此外，OER和UOR的Tafel斜率分别为40.2和58.3 mV/dec，表明动力学增强和催化性能优越。此外，对催化剂进行的稳定性测试表明，Ce-NiS2@CC具有优异的电化学长期稳定性，使其成为各种应用中高度可靠和耐用的选择。密度泛函理论计算和原位拉曼结果表明，Ce掺杂和硫空位协同促进表面重构形成NiⅢ-O物质，调节Ni位点附近的局部电荷分布，从而促进水分子的吸附和活化，从而加速OER动力学。本研究系统研究了金属掺杂和空位缺陷对电催化性能的影响，为高效电催化剂的电子结构调控和性能优化提供了新的思路。

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引用次数: 0

Oxygen radical coupling on asymmetric Ni-Co dual-sites induced by rare earth hydroxides for enhanced alkaline oxygen evolution reaction 稀土氢氧化物诱导非对称Ni-Co双位点氧自由基偶联增强碱性析氧反应

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.03.019

Jiamin Zhu , Shuhui Li , Yue Zhai , Zejin Lin , Jingzhi Yang , Shanshan Wu , Nan Zhang , Li An , Pinxian Xi , Chun-Hua Yan

The reaction pathway plays a pivotal role in determining the catalytic activity of the oxygen evolution reaction (OER). However, regulating the microscopic reaction pathway through interface construction remains a significant challenge. In this study, an interface between amorphous rare earth hydroxides and crystalline spinel NiCo₂O₄ was constructed via selective oxidation. The interface structural units accelerate reconstruction, leading to enhanced catalytic activity, which was observed by in situ Raman spectroscopy. The amorphous RE(OH)₃ (RE = Y and Eu) optimize asymmetric Ni‒Co dual-sites, thereby altering the OER reaction pathway. Specifically, Y(OH)₃/NiCo₂O₄ operates through the lattice oxygen mechanism (LOM) at the expense of structural stability, whereas Eu(OH)₃/NiCo₂O₄ follows the oxygen pathway mechanism (OPM), preserving both catalytic activity and stability. This study offers a novel approach to controlling reaction pathways and proposes a new strategy for interface construction using rare earth hydroxides.

反应途径是决定析氧反应（OER）催化活性的关键因素。然而，通过界面构建调节微观反应途径仍然是一个重大挑战。在本研究中，非晶稀土氢氧化物和结晶尖晶石NiCo2O4之间通过选择性氧化建立了一个界面。通过原位拉曼光谱观察到，界面结构单元加速了重建，导致催化活性增强。无定形RE(OH)3 （RE = Y和Eu）优化了不对称Ni-Co双位点，从而改变了OER反应途径。具体来说，Y(OH)3/NiCo2O4通过晶格氧途径机制（LOM）运行，以牺牲结构稳定性为代价，而Eu(OH)3/NiCo2O4遵循氧途径机制（OPM），保持了催化活性和稳定性。本研究提供了一种控制反应途径的新方法，并提出了一种利用稀土氢氧化物构建界面的新策略。

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引用次数: 0

Nitrogen doped carbon nanotube confined rare earth oxide-alloy heterostructure for efficient electrocatalytic water dissociation 氮掺杂碳纳米管约束稀土氧化物合金异质结构的高效电催化水解离

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths

Pub Date : 2026-02-01 DOI: 10.1016/j.jre.2025.02.024

Yong Jiang , Qiang Wang , Yaping Du

It is crucial to design highly active, durable, and low precious metal mass-loaded hydrolysis ionization catalysts to promote slow water dissociation for hydrogen production. Herein, a series of armor-like catalyst heterogeneous structures of rare earth (RE) oxide/alloy confined within carbon nanotubes (RuCo/CeO₂-NCNTs) was prepared using a one-step pyrolysis phase separation strategy. The prepared catalysts need only overpotentials of 12 and 51 mV for hydrogen evolution reaction (HER) and 141 and 192 mV for oxygen evolution reaction (OER) to achieve a current density of 10 mA/cm² in 1.0 mol/L KOH and 0.5 mol/L H₂SO₄ electrolytes. Under alkaline conditions, both HER and OER can work steadily for 1000 h. The turnover frequency (TOF) values of HER and OER are 33.08 s⁻¹ (@100 mV) and 12.75 s⁻¹ (@300 mV) in alkaline environments, respectively. The in situ electrochemical impedance spectroscopy (EIS) test results further confirm that the introduction of cerium oxide optimizes the mass transfer process during the electrochemical process and enhances catalytic activity. The synergistic effect of the RuCo and CeO₂ heterostructure confined within NCNTs, combined with the increased conductivity resulting from the expansion of the conductive channels, accelerates reaction kinetics and enhances performance. This study also demonstrates the confinement of RE oxide heterostructures within NCNTs, providing a new solution for the development of novel RE-based catalysts and the high-value utilization of RE.

设计高活性、耐用、低贵金属质量负载的水解电离催化剂是促进水缓慢解离制氢的关键。本文采用一步热解相分离策略制备了一系列限制在碳纳米管（RuCo/CeO2-NCNTs）内的非均相结构稀土氧化物/合金类盔甲催化剂。制备的催化剂在1.0 mol/L KOH和0.5 mol/L H2SO4电解质中，析氢反应（HER）的过电位为12和51 mV，析氧反应（OER）的过电位为141和192 mV，电流密度为10 mA/cm2。在碱性条件下，HER和OER的TOF值分别为33.08 s−1 （@100 mV）和12.75 s−1 (@300 mV)，均可稳定工作1000 h。原位电化学阻抗谱（EIS）测试结果进一步证实了氧化铈的引入优化了电化学过程中的传质过程，提高了催化活性。限制在NCNTs内的RuCo和CeO2异质结构的协同效应，加上导电通道扩张导致的电导率增加，加速了反应动力学并提高了性能。该研究还证明了稀土氧化物异质结构在NCNTs内的限制，为新型稀土基催化剂的开发和稀土的高价值利用提供了新的解决方案。

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