Chinese Journal of Catalysis最新文献_第3页

Photocatalyzed C–N coupling reactions of small molecules 光催化小分子C-N偶联反应

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-01-01 DOI: 10.1016/S1872-2067(25)64838-8

Lin-Xing Zhang , Chang-Long Tan , Ming-Yu Qi , Zi-Rong Tang , Yi-Jun Xu

Catalytic coupling of abundant CO₂ or renewable CH₃OH with nitrogenous small molecules, such as N₂, NH₃, and NO₃⁻, has emerged as a promising strategy for synthesizing high-value organonitrogen compounds. However, conventional thermal catalysis for C–N bond formation often relies on external chemical reagents and energy-intensive conditions, raising concerns about process sustainability. Photocatalysis offers a sustainable alternative by utilizing sunlight to generate high-energy electron-hole pairs in semiconductors, which can activate inert chemical bonds (e.g., C=O and N≡N) for programmed coupling under ambient conditions. In this review, we dissect the fundamental activation mechanisms underlying photon-mediated C‒N coupling reactions, highlight key recent breakthroughs in the synthesis of urea, formamide, and amino acids, and analyze persistent challenges alongside emerging opportunities. This work aims to deepen the understanding of photocatalytic C–N coupling reactions and inspire research interest in sustainable nitrogen fixation and carbon utilization.

丰富的CO2或可再生的CH3OH与含氮小分子（如N2、NH3和NO3−）的催化偶联已成为合成高价值有机氮化合物的一种有前途的策略。然而，传统的C-N键形成的热催化通常依赖于外部化学试剂和能源密集型条件，这引起了对过程可持续性的担忧。光催化提供了一种可持续的替代方案，利用阳光在半导体中产生高能电子-空穴对，这可以激活惰性化学键（例如，C=O和N≡N），在环境条件下进行程序化耦合。在这篇综述中，我们剖析了光子介导的C-N偶联反应的基本激活机制，重点介绍了尿素、甲酰胺和氨基酸合成方面的最新突破，并分析了持续存在的挑战和新兴的机遇。这项工作旨在加深对光催化C-N偶联反应的理解，激发对可持续固氮和碳利用的研究兴趣。

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引用次数: 0

Alkali cation effects in electrochemical carbon dioxide reduction 碱阳离子在电化学二氧化碳还原中的作用

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-01-01 DOI: 10.1016/S1872-2067(25)64834-0

Jiaqi Xiang , Limiao Chen , Shanyong Chen , You-Nian Liu

In recent decades, the unabated consumption of fossil fuels has resulted in a sustained increase in carbon dioxide emissions, exacerbating environmental challenges typified by the greenhouse effect, which has underscored the urgent imperative to develop highly efficient carbon dioxide capture and utilization technologies. The electrocatalytic carbon dioxide reduction reaction (eCO₂RR) has emerged as a promising strategy for the conversion of CO₂ into high-value-added chemical commodities. Recent investigations have demonstrated that alkali cations played a pivotal role in eCO₂RR, encompassing enhancements in catalytic activity and modulations of product selectivity. Despite these advancements, how exactly the alkali cations affect the electrocatalytic reaction process and the key determinants of alkali cation effects remain subjects of ongoing debate. We analyzed current research on the effects of alkali cations, in which the concentration and type of alkali cations were generally correlated with eCO₂RR performance. However, the distribution of alkali cations at the electrode interface is often overlooked. In this study, we first conclude recent advancements in electric double layer theory and elucidate three distinct modes of alkali cation distribution at the electrode-electrolyte interface. Subsequently, we systematically summarize the specific mechanisms through which these cations operate in different electrolyte systems. Furthermore, we propose fundamental perspectives for future investigations into alkali cation effects, aiming to provide guiding principles for the rational design of next-generation advanced eCO₂RR electrolysis systems.

近几十年来，化石燃料的持续消耗导致二氧化碳排放量持续增加，加剧了以温室效应为代表的环境挑战，这凸显了开发高效二氧化碳捕获和利用技术的紧迫性。电催化二氧化碳还原反应（eCO2RR）已成为将二氧化碳转化为高附加值化学商品的一种有前途的策略。最近的研究表明，碱离子在eCO2RR中发挥了关键作用，包括催化活性的增强和产物选择性的调节。尽管取得了这些进展，碱阳离子究竟如何影响电催化反应过程以及碱阳离子效应的关键决定因素仍然是持续争论的主题。我们分析了目前关于碱阳离子影响的研究，碱阳离子的浓度和类型通常与eCO2RR性能相关。然而，碱阳离子在电极界面的分布往往被忽视。在这项研究中，我们首先总结了电双层理论的最新进展，并阐明了碱阳离子在电极-电解质界面上的三种不同的分布模式。随后，我们系统地总结了这些阳离子在不同电解质体系中作用的具体机制。此外，我们对碱阳离子效应的未来研究提出了基本观点，旨在为下一代先进的eCO2RR电解系统的合理设计提供指导原则。

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引用次数: 0

Dual-site confinement strategy tuning Fe-N-C electronic structure to enhance oxygen reduction performance in PEM fuel cells 双位约束策略调整Fe-N-C电子结构以提高PEM燃料电池的氧还原性能

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-01-01 DOI: 10.1016/S1872-2067(25)64804-2

Wenbo Shi , Kai Zhu , Xiaogang Fu , Chenhong Liu , Yang Yuan , Jialiang Pan , Qing Zhang , Zhengyu Bai

Single atomic iron-nitrogen-carbon (Fe-N-C) have emerged as promising catalysts for the oxygen reduction reaction (ORR), however, the insufficient activity and stability hindered their application in proton exchange membrane fuel cells (PEMFCs). Simultaneously regulating the coordination environments and local carbon structures of atomic Fe-N sites is essential to boost Fe-N-C's ORR performance. In this study, a dual-site confinement strategy is proposed to precisely incorporate Mn single atoms at adjacent Fe sites to form active and stable FeMn-N catalytic structure within a graphitic carbon matrix, which is achieved via heat treatment of MnFe₂O₄ nanoparticles embedded ZIF-8. Experimental and theoretical calculations demonstrate that the incorporation of Mn atoms could effectively modulate the electronic structure of Fe atoms, enhance Fe–N bond stability and reduce Fe site dissolution. Moreover, in-situ Raman and in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy spectra suggest that Mn doping could suppress Fenton reactions by optimizing the ORR pathway through facilitating *OH intermediate desorption and circumventing *OOH intermediate formation. The synthesized FeMn-N-C exhibits better catalytic activity than commercial Pt/C catalysts (E_1/2 of 0.885 vs. 0.855 V) and maintains stable cycling operation over 20000 cycles with a small E_1/2 gap of 95 mV. When applied in PEMFCs, FeMn-N-C achieves a high peak power density of 899.9 mW cm⁻² and retains 66.4% of its initial performance after 20000 square-wave cycles, which is superior to Fe-N-C catalyst. This study provides an innovative design strategy for developing high-performance, long-lasting ORR catalysts for PEMFCs.

单原子铁-氮-碳（Fe-N-C）已成为氧还原反应（ORR）的催化剂，但其活性和稳定性不足阻碍了其在质子交换膜燃料电池（pemfc）中的应用。同时调节Fe-N原子位的配位环境和局部碳结构对提高Fe-N- c的ORR性能至关重要。在本研究中，提出了一种双位点约束策略，通过热处理嵌入ZIF-8的MnFe2O4纳米颗粒，将Mn单原子精确地结合在相邻的Fe位点上，在石墨碳基体内形成活性稳定的FeMn-N催化结构。实验和理论计算表明，Mn原子的掺入可以有效地调节Fe原子的电子结构，增强Fe - n键的稳定性，减少Fe位点的溶解。此外，原位拉曼光谱和原位衰减全反射表面增强红外吸收光谱表明，Mn掺杂可以通过促进*OH中间体解吸和规避*OOH中间体形成来优化ORR途径，从而抑制Fenton反应。合成的FeMn-N-C催化剂的催化活性优于商用Pt/C催化剂（E1/2为0.885 vs. 0.855 V），在20000次循环中保持稳定的循环运行，e2 /2间隙很小，为95 mV。当FeMn-N-C应用于pemfc时，经过20000次方波循环，FeMn-N-C的峰值功率密度达到899.9 mW cm - 2，保持了66.4%的初始性能，优于Fe-N-C催化剂。该研究为开发高性能、长效的pemfc ORR催化剂提供了一种创新的设计策略。

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引用次数: 0

S-scheme heterojunctions of metal-doped ZnIn2S4/TpPa-1: Regulating H adsorption/desorption and internal electric field for boosted dual-functional photocatalysis 金属掺杂ZnIn2S4/TpPa-1的s型异质结：调节H吸附/解吸和增强双功能光催化的内部电场

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-01-01 DOI: 10.1016/S1872-2067(25)64879-0

Shaodan Wang , Heng Yang , Lijun Xue , Jianjun Zhang , Shuxin Ouyang , Lili Wen

Cooperative coupling of photocatalytic hydrogen generation with oxidative organic synthesis is promising in simultaneously producing sustainable energy and value-added chemicals. However, the photocatalytic activity is constrained by restricted redox potentials and insufficient photocarrier separation and transfer. Herein, we construct S-scheme heterojunctions based on metal-doped ZnIn₂S₄ and covalent organic frameworks, denoted as M-ZIS/TpPa-1 (M = Ni or Mo). Theoretical calculations demonstrated that Mo-ZIS possess optimum H adsorption Gibbs free energies, deeper downshift of sulfur p-band center and higher integrated crystal orbital Hamilton population (ICOHP) value than Ni-ZIS and ZIS to optimize H adsorption/desorption dynamics. Besides, metal-doping reasonably enhanced the interfacial charge transfer in heterostructures, identifying the enlarged internal electric field (IEF) in Mo-ZIS/TpPa-1 than Ni-ZIS/TpPa-1 and ZIS/TpPa-1. Moreover, experimental explorations of photoelectrochemical measurements, femtosecond transient absorption spectroscopy, in-situ irradiated X-ray photoelectron spectroscopy and electron paramagnetic resonance verified the facilitated photocarrier separation and migration in metal-doped S-scheme heterojunctions. Ultimately, Mo_0.01-ZIS/TpPa-1 exhibited visible-light driven H₂ evolution rate of 1648 μmol g⁻¹ h⁻¹ and N-benzylidenebenzylamine formation rate of 1812 μmol g⁻¹ h⁻¹, better than Ni_0.048-ZIS/TpPa-1, and superior to parent ZIS/TpPa-1. This work might provide insights into the modulation of H adsorption/desorption behavior and IEF within S-scheme heterostructures via rational metal-doping strategy for efficient dual-functional photocatalysis.

光催化制氢与氧化有机合成的协同耦合在同时生产可持续能源和增值化学品方面具有广阔的前景。然而，光催化活性受到氧化还原电位受限和光载流子分离和转移不足的限制。在这里，我们构建了基于金属掺杂ZnIn2S4和共价有机框架的s方案异质结，记为M- zis /TpPa-1 （M = Ni或Mo）。理论计算表明，与Ni-ZIS和ZIS相比，Mo-ZIS具有最佳的H吸附吉布斯自由能、更深的硫p带中心下移和更高的集成晶体轨道汉密尔顿居群（ICOHP）值，从而优化H吸附/解吸动力学。此外，金属掺杂合理地增强了异质结构中的界面电荷转移，发现Mo-ZIS/TpPa-1的内部电场（IEF）比Ni-ZIS/TpPa-1和ZIS/TpPa-1的内部电场（IEF）更大。此外，光电化学测量、飞秒瞬态吸收光谱、原位辐照x射线光电子能谱和电子顺磁共振的实验探索证实了在金属掺杂的S-scheme异质结中促进光载流子的分离和迁移。最终，Mo0.01-ZIS/TpPa-1的可见光驱动H2进化速率为1648 μmol g−1 h−1，n -苄基苯胺生成速率为1812 μmol g−1 h−1，优于Ni0.048-ZIS/TpPa-1，优于亲本ZIS/TpPa-1。这项工作可能为通过合理的金属掺杂策略调节S-scheme异质结构中的H吸附/解吸行为和IEF提供新的见解，以实现高效的双功能光催化。

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引用次数: 0

Key components for realistic application of plastic photoreforming coupled with H2 evolution 塑料光重整耦合析氢实际应用的关键部件

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-01-01 DOI: 10.1016/S1872-2067(25)64869-8

Jinpeng Zhang , Teng Liang , Jaenudin Ridwan , Tian Chen , Elhussein M. Hashem , Meijun Guo , Amin Talebian-Kiakalaieh , Le Yu , Ping She , Jingrun Ran

Green hydrogen (H₂) energy plays an important role in combating climate change, promoting energy transition, and fostering sustainable development. Solar-driven plastic photoreforming afford an attractive solution, it overcomes the limitation of the slow oxygen evolution half-reaction in overall water splitting while tackling environmental pollution and resource waste caused by plastics. However, this technology still rests on the experimental stage, and the transition from laboratory to realistic application remains lacking systematic view. In this review, key components for plastic photoreforming, including plastic pretreatment routes, photocatalysts exploration, basic photocatalytic modules for the realistic application, and feasibility, are investigated. Finally, outlook in this area is discussed.

绿色氢能在应对气候变化、促进能源转型、促进可持续发展方面发挥着重要作用。太阳能驱动的塑料光重整提供了一种很有吸引力的解决方案，它克服了整体水分解中析氧半反应缓慢的局限性，同时解决了塑料造成的环境污染和资源浪费。然而，该技术还停留在实验阶段，从实验室到现实应用的过渡还缺乏系统的认识。本文综述了塑料光重整的关键技术，包括塑料预处理路线、光催化剂的开发、基本光催化模块的实际应用及其可行性。最后，对该领域的发展前景进行了展望。

引用次数: 0

Grain boundary engineering of CeO2 induced electron redistribution for dimethyl carbonate synthesis from CO2 CO2合成碳酸二甲酯中CeO2诱导电子重分布的晶界工程

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-01-01 DOI: 10.1016/S1872-2067(25)64871-6

Guoqiang Hou, Di Xu, Haifeng Fan, Yangyang Li, Siyi Huang, Mingyue Ding

Direct synthesis of dimethyl carbonate (DMC) from CO₂ is critical for achieving carbon neutrality, yet the sluggish formation and conversion of the key *CH₃OCOO intermediate-due to the difficulty of C-O coupling-limit high DMC yields. Herein, we developed a boric acid-assisted recrystallization strategy to fabricate grain-boundary-rich CeO₂ hollow nanospheres, which serve as an efficient catalyst for CO₂ to DMC synthesis. The introduction of grain-boundary (GBs) induced the electron redistribution, which led a decrease in the electron density of bulk Ce ions and created a localized electron-rich region at homogeneous interface. This unique electronic landscape promoted reactive methoxy formation and stronger CO₂ adsorption, thereby enabling more efficient coupling of *CH₃O and *CO₂ to form the *CH₃OCOO. Concurrently, the enhanced CO₂ adsorption facilitated the dissociation of *CH₃OCOO and subsequent DMC formation. As a result, the 4%BCeO₂-GBs achieved an advantageous DMC yield of 19.8 mmol/g. In the assistance of dehydrating agent, the catalyst delivered a remarkable 264.2 mmol/g DMC yield and 7.12% methanol conversion, which was 32 times higher than commercial CeO₂. This study elucidated the intrinsic mechanisms governing *CH₃OCOO intermediate behavior and offers valuable guidance for CO₂ converting into high-value organic chemicals.

由二氧化碳直接合成碳酸二甲酯（DMC）对于实现碳中和至关重要，但由于C-O偶联困难，关键的*CH₃OCOO中间体的形成和转化缓慢，限制了DMC的高产率。在此，我们开发了硼酸辅助重结晶策略来制备富晶界的CeO2空心纳米球，作为CO2合成DMC的有效催化剂。晶界（GBs）的引入引起了电子重分布，导致大块Ce离子的电子密度降低，并在均匀界面处形成局域富电子区。这种独特的电子景观促进了反应性甲氧基的形成和更强的CO2吸附，从而使* ch30和*CO2更有效地偶联形成*CH3OCOO。同时，CO2吸附的增强促进了*CH3OCOO的解离和随后的DMC的形成。结果表明，4%BCeO2-GBs的DMC产率为19.8 mmol/g。在脱水剂的辅助下，该催化剂的DMC产率为264.2 mmol/g，甲醇转化率为7.12%，是商品CeO2的32倍。该研究阐明了*CH3OCOO中间体行为的内在机制，为CO2转化为高价值有机化学品提供了有价值的指导。

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引用次数: 0

Construction of Ag single atoms and nanoparticles co-modified g-C3N4 for synergistic plasma photocatalytic broad-spectrum hydrogen production Ag单原子和纳米粒子共修饰g-C3N4协同等离子体光催化广谱制氢的构建

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-11-17 DOI: 10.1016/S1872-2067(25)64846-7

Weijie Zhan, Nan Yang, Tong Zhou, Jin Zhang, Tianwei He, Qingju Liu

Solar-driven water splitting has emerged as a promising route for sustainable hydrogen generation, however, developing broad-spectrum responsive photocatalysts remains a challenge for achieving efficient solar-to-hydrogen conversion. Here, we demonstrate a g-C₃N₄ -based (UCN) catalyst with dispersed Ag single atoms (Ag SAs) and Ag nanoparticles (Ag NPs) for synergistically broad-spectrum photocatalytic hydrogen evolution. Experimental and theoretical results reveal that both Ag SAs and Ag NPs serve as active sites, with the Schottky junction between Ag NPs and g-C₃N₄ effectively promoting charge separation, while Ag NPs induce localized surface plasmon resonance, extending the light response range from visible to near-infrared regions. The optimized catalyst Ag-UCN-3 exhibits a hydrogen evolution rate as high as 22.11 mmol/g/h and an apparent quantum efficiency (AQE) of 10.16% under 420 nm light illumination. Notably, it still had a high hydrogen evolution rate of 633.57 μmol/g/h under 700 nm irradiation. This work unveils dual active sites engineering strategy that couples Ag SAs and Ag NPs with plasma and hot electrons, offering a new strategy for designing high-performance solar-driven energy systems.

太阳能驱动的水分解已经成为可持续制氢的一种有前途的途径，然而，开发广谱反应性光催化剂仍然是实现高效太阳能制氢转化的一个挑战。在这里，我们展示了一种基于g-C3N4 （UCN）的催化剂，该催化剂具有分散的Ag单原子（Ag SAs）和Ag纳米粒子（Ag NPs），用于协同广谱光催化析氢。实验和理论结果表明，Ag sa和Ag NPs都是活性位点，Ag NPs与g-C3N4之间的肖特基结有效地促进了电荷分离，而Ag NPs诱导局部表面等离子体共振，将光响应范围从可见光区扩展到近红外区。优化后的Ag-UCN-3催化剂在420 nm光照下的析氢速率高达22.11 mmol/g/h，表观量子效率（AQE）为10.16%。值得注意的是，在700 nm辐照下，其析氢速率仍然很高，达到633.57 μmol/g/h。这项工作揭示了将Ag sa和Ag NPs与等离子体和热电子耦合的双活性位点工程策略，为设计高性能太阳能驱动能源系统提供了一种新的策略。

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引用次数: 0

S-scheme Cd0.8Zn0.2S nanowires/CeO2 nanocubes heterojunction for efficient photocatalytic hydrogen evolution S-scheme Cd0.8Zn0.2S纳米线/CeO2纳米立方异质结高效光催化析氢

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-11-17 DOI: 10.1016/S1872-2067(25)64843-1

Yuqing Yan , Yonghui Wu , Jun Wang , Jinrong Huo , Kai Yang , Kangqiang Lu

Constructing S-scheme heterojunctions preserves the intrinsic redox capabilities of both semiconductors while promoting the separation of photogenerated electrons and holes, making it a promising approach for enhancing the properties of semiconductors. In this study, an S-scheme Cd_0.8Zn_0.2S-CeO₂ (CZS-CeO₂) heterojunction was successfully fabricated via the in-situ growth of CZS nanowires on CeO₂ nanocubes. The S-scheme charge-transfer mechanism of the CZS-CeO₂ composites during photocatalytic reactions was confirmed through in-situ X-ray photoelectron spectroscopy and density functional theory calculations. These results demonstrate that the interfacial electric field (IEF) significantly facilitates charge separation and transport within the heterojunction. Consequently, the CZS-CeO₂ composites exhibited excellent photocatalytic hydrogen production performance under simulated sunlight irradiation, surpassing that of blank CZS. Particularly, the optimal photocatalytic hydrogen generation rate for CZS-15%CeO₂ reached 58 mmol·g^–1·h^–1, approximately 8.8 times higher than that of blank CZS. After five consecutive cycles of testing, CZS-15%CeO₂ retained a relatively high level of activity. This enhanced stability can be attributed to the fabrication of S-scheme heterojunctions, which effectively suppressed hole-induced photocorrosion of CZS. This investigation provides a beneficial reference for the rational design of S-scheme heterojunction photocatalysts for efficient and stable photocatalytic hydrogen production.

构建S-scheme异质结保留了两种半导体的固有氧化还原能力，同时促进了光生电子和空穴的分离，使其成为提高半导体性能的一种有前途的方法。在本研究中，通过在CeO2纳米立方上原位生长cjs纳米线，成功制备了S-scheme Cd0.8Zn0.2S-CeO2 （cjs -CeO2）异质结。通过原位x射线光电子能谱和密度泛函理论计算，证实了cjs - ceo2复合材料在光催化反应中的S-scheme电荷转移机理。这些结果表明，界面电场（IEF）显著促进了异质结内电荷的分离和输运。结果表明，cjs - ceo2复合材料在模拟阳光照射下表现出优异的光催化制氢性能，优于空白cjs。其中，cjs -15% ceo2的最佳光催化产氢速率达到58 mmol·g-1·h-1，是空白cjs的8.8倍左右。经过连续五个周期的测试，cjs -15% ceo2保持了相对较高的活性水平。这种增强的稳定性可以归因于S-scheme异质结的制备，它有效地抑制了cjs的空穴诱导光腐蚀。该研究为合理设计s型异质结光催化剂，实现高效稳定的光催化制氢提供了有益的参考。

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引用次数: 0

Unlocking 5300-h ultrastable metal-free ORR catalysts for Zn-air batteries via F–N co-doped tailored carbon pore architectures and synergistic adsorption modulation 通过F-N共掺杂定制碳孔结构和协同吸附调制解锁锌空气电池5300-h超稳定无金属ORR催化剂

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-11-17 DOI: 10.1016/S1872-2067(25)64835-2

Baofa Liu , Weijie Pan , Zhiyang Huang , Yi Zhao , Zuyang Luo , Tayirjan Taylor Isimjan , Bao Wang , Xiulin Yang

Designing exceptional-performance and long-lasting oxygen reduction reaction (ORR) catalysts is a critical challenge for the development of rechargeable Zn-air batteries (ZABs). In this study, we introduce a metal-free ORR catalyst composed of F–N co-doped hollow carbon (FNC), specifically engineered to address the limitations of conventional catalysts. The FNC catalysts were synthesized using a template-assisted pyrolysis method, resulting in a hollow, porous architecture with a high specific surface area and numerous active sites. Concurrently, F doping optimized the electronic configuration of pyridinic nitrogen. The introduction of C–F bonds reduced the reaction energy barrier, and the resulting N-C-F configuration enhanced the stability of the nitrogen center. The catalyst exhibits outstanding ORR activity in alkaline media, exhibiting a half-wave potential (E_1/2) of 0.87 V, surpassing that of commercial Pt/C (E_1/2 = 0.85 V). When applied to both aqueous and flexible ZAB configurations, the FNC catalyst achieved peak power densities of 172 and 85 mW cm^–2, respectively, along with exceptional cycling stabilities exceeding 5300 and 302 h, respectively. This study establishes a novel approach for designing metal-free ORR catalysts and next-generation ZABs, particularly for use in flexible and wearable microelectronic devices.

设计高性能、长效的氧还原反应（ORR）催化剂是发展可充电锌空气电池（ZABs）的关键挑战。在这项研究中，我们介绍了一种由F-N共掺杂空心碳（FNC）组成的无金属ORR催化剂，专门设计用于解决传统催化剂的局限性。FNC催化剂采用模板辅助热解法合成，得到了具有高比表面积和大量活性位点的中空多孔结构。同时，F掺杂优化了吡啶氮的电子构型。C-F键的引入降低了反应能垒，生成的N-C-F构型增强了氮中心的稳定性。该催化剂在碱性介质中表现出出色的ORR活性，其半波电位（E1/2）为0.87 V，超过了商用Pt/C （E1/2 = 0.85 V）。当应用于含水和柔性ZAB配置时，FNC催化剂的峰值功率密度分别为172和85 mW cm-2，同时具有出色的循环稳定性，分别超过5300和302小时。本研究建立了一种设计无金属ORR催化剂和下一代ZABs的新方法，特别是用于柔性和可穿戴微电子设备。

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引用次数: 0

In-situ and operando characterizations in membrane electrode assemblies: Resolving dynamic interfaces and degradation pathways in CO2 electrocatalysis 膜电极组件的原位和操作性表征：解决CO2电催化中的动态界面和降解途径

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-11-17 DOI: 10.1016/S1872-2067(25)64820-0

Jiachen Wu, Pengfei Liu, Huagui Yang

Membrane electrode assemblies (MEAs) represent the preeminent configuration for industrial-scale CO₂ electrolysis, yet their dynamic interfaces and degradation pathways remain inadequately resolved. This perspective highlights how advanced operando characterization techniques—synchrotron X-ray spectroscopy, spatially resolved X-ray fluorescence, vibrational spectroscopy, electrochemical diagnostics et al.—decipher atomic-scale catalyst evolution, transient ion/water fluxes, and extreme interfacial microenvironments under industrial current densities. These methodologies reveal critical degradation mechanisms, including catalyst restructuring, carbonate precipitation-driven flooding, and cation-induced pH gradients, which are inaccessible to conventional ex-situ or three-electrode analyses. Integrating multimodal characterization is paramount to correlate transient interfacial chemistry with system-level performance, guiding the rational design of durable, high-selectivity MEAs for scalable CO₂ conversion.

膜电极组件（MEAs）代表了工业规模二氧化碳电解的卓越配置，但其动态界面和降解途径仍未得到充分解决。这一观点强调了先进的operando表征技术——同步加速器x射线光谱、空间分辨x射线荧光、振动光谱、电化学诊断等——如何在工业电流密度下破译原子级催化剂演化、瞬态离子/水通量和极端界面微环境。这些方法揭示了关键的降解机制，包括催化剂重组、碳酸盐沉淀驱动的驱油和阳离子诱导的pH梯度，这些都是传统的非原位或三电极分析无法实现的。整合多模态表征对于将瞬态界面化学与系统级性能相关联至关重要，可以指导合理设计耐用、高选择性的mea，用于可扩展的二氧化碳转化。

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引用次数: 0