Materials Chemistry Frontiers最新文献

{"title":"Steric hindrance of organotin compounds in controlling the batch-to-batch variance of photovoltaic polymer donors†","authors":"Yongrui He, Yuchen Yue, Jingfa Zhang, Ying Huang, Xucong Zhou, Han Shen, Kuan Li, Jie Shen, Landi Zeng, Jingjing Liu, Jingxia Wang, Bin Wang, Lei Jiang, Lijun Huo and Bing Zheng","doi":"10.1039/D5QM00005J","DOIUrl":"https://doi.org/10.1039/D5QM00005J","url":null,"abstract":"<p >Owing to its advantages of mild reaction conditions and a single reaction system, Stille coupling has become the main method of developing high-performance photovoltaic polymers. However, Stille coupling polycondensation, following a step-growth polymerization mechanism, still presents challenges in controlling the molecular weights of the polymers, leading to significant batch-to-batch variance. Herein, a strategy based on steric effects was applied to reduce molecular weight fluctuations using the large steric groups of organotin compounds to increase the difficulty of forming the transmetalation transition state. Consequently, we conducted competition experiments with small molecules and synthesized three polymers (<strong>PDF-1</strong>, <strong>PDF-2</strong>, and <strong>PDF-3</strong>) using BDF-based organotin compounds with varying steric hindrance. Theoretical calculations proved that the steric hindrance of organotin compounds significantly influenced the transition state in the transmetalation process. Device measurements revealed that the larger steric hindrance of organostannides could produce polymers with concentrated molecular weights, resulting in only a slight change in the PCEs. Although excessive steric hindrance could affect the photovoltaic properties, leading to lower PCEs, appropriate steric control of organostannides could yield polymer donors with high performance and low batch-to-batch variance. Therefore, this work provides guidelines for developing polymers with minimal batch-to-batch variance.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 5","pages":" 847-855"},"PeriodicalIF":6.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143480828","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Construction of full-color room-temperature afterglow materials using dicyanomethylene-4H-pyrans based on an alkene conjugated bridge as the third component†","authors":"Jiayin Qian, Wenbo Dai, Xiaoyu Qiu, Shuai Xia, Yunxiang Lei, Miaochang Liu, Yan Guan, Xiaobo Huang and Huayue Wu","doi":"10.1039/D4QM01025F","DOIUrl":"https://doi.org/10.1039/D4QM01025F","url":null,"abstract":"<p >Although the alkene bond as a connecting unit is widely used to construct D–π–A luminescent molecules, room-temperature afterglow (RTA) systems containing this kind of molecule are extremely rare. In this work, a series of multi-component doped RTA materials were prepared using polyvinylpyrrolidone as the host, 2-(4-chlorophenyl)-1-(4-(diphenylamino)phenyl)ethan-1-one as the guest, dicyanomethylene-4<em>H</em>-pyrans with an alkene bond bridge as the third component, and <strong>RhB</strong> and <strong>Cy5</strong> as the fourth component. Two-component materials emit bright cyan room-temperature phosphorescence; three-component materials emit yellow-green, orange, and red afterglows, respectively; and four-component doped materials further exhibit afterglow at 740 nm in the near-infrared region. The RTA emissions of three-component and four-component materials have been shown to be delayed fluorescence, which is caused by the phosphorescence of the second component transitioning from the triplet state to the singlet state and thus the domino-type Förster resonance energy transfer of S<small>₁</small>–S<small>₁</small> between different luminescent molecules. The results reveal that using dicyanomethylene-4<em>H</em>-pyrans as the third component can lead to full-color afterglow emissions. This work gives a possible development direction for the construction of RTA materials using D–π–A fluorescent molecules.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 5","pages":" 818-827"},"PeriodicalIF":6.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143480826","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A strongly coupled FeS2@TiO2 heterostructure with an island-like structure for high-efficiency lithium storage†","authors":"Luchao Yue, Wei Song, Yu Feng, Lixin Zhang, Ruina Shi, Lin Jiang, Jing Song, Guisheng Qi and Xuping Sun","doi":"10.1039/D4QM00675E","DOIUrl":"https://doi.org/10.1039/D4QM00675E","url":null,"abstract":"<p >Titanium dioxide (TiO<small>₂</small>) has garnered substantial interest as a potential anode material for advanced lithium-ion batteries (LIBs) owing to its superior structural stability, rapid pseudocapacitive kinetics, economic viability, and nontoxicity. Nevertheless, its practical application is significantly curtailed by the limitations in specific capacity and inferior intrinsic electronic conductivity. Although carbonaceous materials can enhance electronic conductivity to a certain extent, the deficiency in lithium storage capacity persists as a critical issue requiring amelioration. Herein, we introduce a unique heterostructure composed of TiO<small>₂</small> nanobelts and FeS<small>₂</small> nanoparticles, fabricated through a hydrothermal method, followed by cation exchange and a sulfidation process. For the heterostructure, FeS<small>₂</small> nanoparticles are <em>in situ</em> anchored on the surface of TiO<small>₂</small> nanobelts, forming an island-like p–n heterostructure (FeS<small>₂</small>@TiO<small>₂</small>). The incorporation of FeS<small>₂</small> featuring high specific capacity facilitates the emergence of a built-in electric field at the interface between the two compounds, thereby expediting the charge transport during the lithium storage process. As a consequence, the island-like FeS<small>₂</small>@TiO<small>₂</small> p–n heterostructure delivers a remarkable reversible capacity of 584.9 mA h g<small>⁻¹</small> at 1.0 A g<small>⁻¹</small> after 300 cycles, along with superior rate capability (average capacity of 204.8 mA h g<small>⁻¹</small> at 10.0 A g<small>⁻¹</small>). Even at 5.0 A g<small>⁻¹</small>, the FeS<small>₂</small>@TiO<small>₂</small> anode maintains a substantial specific capacity of 251.2 mA h g<small>⁻¹</small> over 3000 cycles, revealing its outstanding cycling stability. This study suggests that the design strategy coupling TiO<small>₂</small> with other materials that possess high specific capacity could be broadly applied to enhance its electrochemical performance.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 5","pages":" 800-808"},"PeriodicalIF":6.0,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143480824","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Excited-state intramolecular proton transfer derivatives as self-absorption free luminophores for luminescent solar concentrators†","authors":"Phatsathorn Chonlateeroj, Suangsiri Arunlimsawat, Pattarapapa Janthakit, Rattanasiri Wannapakdee, Wijitra Waengdongbung, Taweesak Sudyoadsuk, Pisist Kumnorkaew and Vinich Promarak","doi":"10.1039/D4QM00874J","DOIUrl":"https://doi.org/10.1039/D4QM00874J","url":null,"abstract":"<p >Luminescent solar concentrators (LSCs) have garnered considerable attention for their potential to enhance solar energy harvesting in photovoltaic (PV) systems. However, self-absorption often hinders their efficiency, caused by the overlap between the absorption and emission spectra. Herein, we design, synthesize, and study a series of novel excited-state intramolecular proton transfer (ESIPT) dyes as a new class of self-absorption-free luminophores for efficient transparent LSC-PV devices. <strong>HBTM</strong>, <strong>HBTPM</strong>, and <strong>HBTBP</strong> dyes comprise 2-(benzo[<em>d</em>]thiazol-2-yl)phenol as an electron-donating ESIPT unit functionalized with different π–acceptor moieties of ((3-hexylthiophen-2-yl)methylene)malononitrile, (4-(3-hexylthiophen-2-yl)benzylidene)malononitrile, and (4-(3-hexylthiophen-2-yl)phenyl)(phenyl)methanone, respectively. Theoretical and photophysical analyses confirm the ESIPT nature of these dyes. They show absorption in the UV-blue region and orange-red emissions with large Stokes shifts (4388–10269 cm<small>⁻¹</small>) and decent fluorescence quantum yields (28–47%). Their LSC samples are well prepared by dispersion in a transparent polymethyl methacrylate (PMMA) matrix. The LSC slabs possess good photophysical properties of the dyes with minimal overlap integrals (OI*) of 0.28–1.56% and edge emission efficiencies (<em>η</em><small>_edge</small>) of 47–57%. Photovoltaic performance assessments reveal power conversion efficiencies (PCE) of 0.46% to 0.68% with external photon efficiencies (<em>η</em><small>_ext</small>) of 7.69% for <strong>HBTM</strong>, 6.91% for <strong>HBTPM</strong>, and 2.98% for <strong>HBTBP</strong>. Particularly, <strong>HBTBP</strong>-based LSC exhibits excellent transparency (AVT = 93%; CRI = 97) suitable for window applications. This work represents a significant step toward reducing self-absorption in LSCs while improving photovoltaic performance, paving the way for scalable solar concentrator technologies based on organic materials.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 4","pages":" 695-709"},"PeriodicalIF":6.0,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143379720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Halogenated dibenzoylmethane Eu3+ complexes as spectroscopic markers: a pioneering photobleaching strategy for counterfeit applications and controlling luminescence efficiency†","authors":"Alisia V. Tsorieva, Vladislav M. Korshunov, Mikhail T. Metlin, Tatiana S. Vlasova, Victoria E. Gontcharenko, Daria A. Metlina, Victor O. Kompanets, Sergey V. Chekalin and Ilya V. Taydakov","doi":"10.1039/D4QM00933A","DOIUrl":"https://doi.org/10.1039/D4QM00933A","url":null,"abstract":"<p >A novel method for identifying counterfeit goods based on the difference between photobleaching rates of spectroscopic marker components is proposed. Controlled photobleaching of the dye is achieved <em>via</em> introduction of halogens (I, Cl, Br, and F) into the aromatic moiety of the dibenzoylmethane (DBM) ligand in coordination compounds of Eu<small>³⁺</small>. A spectroscopic marker model that consists of two coordination compounds with different halogens is developed. These compounds exhibit indistinguishable luminescence spectra and emission intensities at low irradiation power. However, exceeding the threshold irradiation power results in rapid photobleaching of the marker fragment derived from the complex with the highest charge number of halogen atoms. This approach introduces new possibilities for quality control of goods that require storage in light-protected environments. The results obtained during the research have both practical and fundamental significance. For the first time, it is established that the halogenation of the DBM ligand leads to the intersystem crossing process termination. Energy of electronic excitation transfers from the singlet excited state to the ion through a charge transfer state instead of the triplet excited state. Such energy transfer pathways sensitize luminescence of Eu<small>³⁺</small> more effectively, resulting in an increase in quantum yield up to 64% upon the introduction of chlorine atoms.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 5","pages":" 809-817"},"PeriodicalIF":6.0,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143480825","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Improving stability and efficiency of PTAA-based inverted perovskite solar cells through a guest strategy†","authors":"Jieying Cao, Xinxing Yin, Lei Lu, Jiaxing Song, Lin Hu, Yingzhi Jin, Zhen Su, Zaifang Li and Jiefeng Hai","doi":"10.1039/D4QM00917G","DOIUrl":"https://doi.org/10.1039/D4QM00917G","url":null,"abstract":"<p >Although poly[bis(4-phenyl) (2,4,6-trimethylphenyl)amine] (PTAA) has been extensively investigated as a hole transport material, its performance regarding stability and efficiency still encounters challenges. In this study, through the introduction of a novel guest molecule BQ-BO, the energy level configuration, hole transport, and interface passivation of PTAA have been significantly enhanced. The large conjugated electron-deficient core and methoxy-substituted triphenylamine arm structure of BQ-BO not only optimize the HOMO energy level but also enhance the hole mobility and conductivity, attaining a photoelectric conversion efficiency of 21.81%. It also exhibited outstanding thermal stability, maintaining an initial efficiency of 90% after 1000 hours of continuous heating at 85 °C, in contrast to a pure PTAA-based device whose efficiency dropped to 70% after 400 hours.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 4","pages":" 658-665"},"PeriodicalIF":6.0,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143379716","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Silicoaluminophosphate-seeded Al-pair-enriched low-silica CHA zeolites for enhanced Sr2+ capture†","authors":"Yufei Wang, Haopeng Su, Shuang Liu, Junyao Pan, Haoyang Zhang, Xue Ding, Yuxin Yan, Keyan Jin, Binyu Wang and Wenfu Yan","doi":"10.1039/D4QM01030B","DOIUrl":"https://doi.org/10.1039/D4QM01030B","url":null,"abstract":"<p >Radioactive strontium-90 (<small>⁹⁰</small>Sr<small>²⁺</small>) in wastewater poses a significant threat to both the environment and living organisms. Conventional treatment strategies, such as ion-exchange resins followed by cement solidification, can still carry the risk of leakage under certain conditions. Low-silica zeolites have demonstrated strong cation sorption capabilities, with <strong>CHA</strong> zeolites showing particular promise for nuclear wastewater treatment. However, synthesizing low-silica <strong>CHA</strong> zeolites with Si/Al ratios around 2 typically requires fluorides or complex crystallization processes. In this study, we present a one-step, fluoride-free synthesis method for low-silica <strong>CHA</strong> zeolites using the silicoaluminophosphate (SAPO) zeolite SAPO-35 as the seed. The SAPO-seeded synthesis method enhances the formation of Al-pairs within the <strong>CHA</strong> framework by releasing partially connected Si and Al species from the SAPO seed. This significantly improves the zeolite's capability to capture the divalent Sr<small>²⁺</small>. The resulting zeolite exhibits a 10% higher Sr<small>²⁺</small> sorption capacity per ion-exchange site compared to <strong>CHA</strong> zeolites synthesized without the SAPO seed. The synthesized zeolite exhibits exceptional Sr<small>²⁺</small> removal efficiency across dosages of 1/50–1/500 g mL<small>⁻¹</small> and the pH range of 3–12. At temperatures of 25 °C, 60 °C, and 80 °C, the sorption capacities reach 112 mg g<small>⁻¹</small>, 144 mg g<small>⁻¹</small>, and 186 mg g<small>⁻¹</small>, respectively. This work highlights the potential of SAPO-seeded synthesis as a practical and scalable approach for producing Al-pair-enriched, low-silica <strong>CHA</strong> zeolites, indicating the high effectiveness for removing <small>⁹⁰</small>Sr<small>²⁺</small> from nuclear wastewater and offering a promising solution for radioactive wastewater management.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 4","pages":" 666-675"},"PeriodicalIF":6.0,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143379717","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-performance MOF-based electromagnetic wave absorption materials: design and performance optimization","authors":"Xiao-Xuan Fan, Zhan-Zhan Wang, Xin-Ci Zhang, Lin Li and Mao-Sheng Cao","doi":"10.1039/D4QM01054J","DOIUrl":"https://doi.org/10.1039/D4QM01054J","url":null,"abstract":"<p >In recent years, the issue of increasing electromagnetic pollution has posed significant challenges for researchers in the field of electromagnetic dissipation, highlighting the urgent need for effective solutions. Metal–organic frameworks (MOFs) have garnered considerable attention due to their compositional designability, large specific surface area, and tunable chemical structure, making them highly desirable precursors for electromagnetic wave absorption materials (EMWAMs). MOF-based EMWAMs exhibit remarkable performance advantages, such as lightweight properties, high loss capability, and a wide effective absorption bandwidth. These advantages are primarily attributed to their excellent impedance matching and multiple attenuation mechanisms. This paper provides a concise discussion on the relationship between the mechanisms and microstructure of EMWAMs. The research progress of MOF-based EMWAMs in recent years is reviewed, including the classification of MOF and MOF composite precursors, design principles and preparation methods. Finally, the problems, challenges and future opportunities of MOF-based EMWAMs are presented. We aim for this review to offer new insights into the design and fabrication of MOF-based EMWAMs, thereby enhancing both the fundamental understanding and practical application of these materials.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 3","pages":" 403-417"},"PeriodicalIF":6.0,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dual role of lone pair electron and rattling vibration in Zintl phase BaCaPb thermoelectric material†","authors":"Shuwei Tang, Pengfei Zhang, Da Wan, Xiaodong Li, Peng Ai, Zhiwei Zhang, Wanrong Guo, Shulin Bai and Xiuling Qi","doi":"10.1039/D4QM00972J","DOIUrl":"https://doi.org/10.1039/D4QM00972J","url":null,"abstract":"<p >The crystal structure, phonon dispersion curves, electronic transport parameters, and thermoelectric (TE) properties of the Zintl phase BaCaPb compound are investigated by first-principles calculations in combination with a two-channel model. The regular residuals analysis demonstrates the crucial role of four-phonon scattering behavior in evaluating the thermal transport properties of the BaCaPb compound on account of the noticeable optical–optical gap. The origin of the rattling vibration behaviour is investigated by the quantitative analysis of chemical bond. The diffusion-like phonons are predominantly influenced by the rattling vibration of the Ba atom in the BaCaPb compound. Moreover, the dual role of the lone electrons in Pb and the rattling vibration of the Ba atom contributes to the ultralow lattice thermal conductivity (1.46 W m<small>⁻¹</small> K<small>⁻¹</small>@ 300 K) in the BaCaPb compound. In addition, the TE properties of the BaCaPb compound are evaluated in consideration of multiple carrier scatterings, and optimal figures of merit (<em>ZT</em>s) of 1.7 and 1.0 are achieved for the <em>n</em>-type and <em>p</em>-type BaCaPb compounds at 600 K. The present work not only reveals the excellent TE properties of the Zintl phase BaCaPb compound through an in-depth study of their thermal and electronic transport properties, but also adopts a two-channel model for the theoretical design of high-efficiency TE materials.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 4","pages":" 592-607"},"PeriodicalIF":6.0,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143379675","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Bifunctional CuNi-x nano-alloys for electrocatalytic nitrate reduction and HPAM oxidation coupling reactions†","authors":"Lijie Qi, Yu Fu, Borui Ji, Bauyrzhan Sarsenbekuly, Wanli Kang, Hongbin Yang and Shujun Liu","doi":"10.1039/D4QM00962B","DOIUrl":"https://doi.org/10.1039/D4QM00962B","url":null,"abstract":"<p >Electrochemical synthesis of ammonia (NH<small>₃</small>) through cathodic nitrate reduction presents an effective alternative to the Haber–Bosch process, enabling efficient ammonia production without significant environmental pollution. The electrocatalytic degradation strategy is an efficient and environmentally friendly tool for the treatment of oily wastewater containing partially hydrolized polyacrylamide (HPAM). Thus, coupling cathodic nitrate reduction with anodic HPAM oxidation can further enhance ammonia synthesis efficiency and HPAM degradation efficiency. Here, we reported an N-doped carbon nanotube loaded with CuNi-<em>x</em> (<em>x</em> = 0.5, 1, 2) as an electrocatalyst for cathodic nitrate reduction coupled with anodic HPAM oxidative degradation. Notably, the CuNi-1 variant achieved the highest ammonia yield of 4962.76 ± 40.22 μg h<small>⁻¹</small> mg<small>_cat</small><small>⁻¹</small> and a faradaic efficiency of 85.91 ± 0.42%. Furthermore, the oxidative degradation rate of HPAM reached a maximum of 81.91 ± 0.36% within 2 h. Anodic HPAM oxidation not only promotes cathodic nitrate reduction but also enables the acquisition of valuable anodic products. Using <em>in situ</em> ATR-SEIRAS, <em>in situ</em> DEMS, and DFT calculations, we thoroughly analyzed reaction intermediates and the critical role of the CuNi bimetallic system in electrocatalytic nitrate reduction. The coupled reaction system was established to achieve both efficient ammonia synthesis and HPAM degradation.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 4","pages":" 638-647"},"PeriodicalIF":6.0,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143379714","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}