Taotao Chu, Mengke Fan, Yu Guo, Meiling Liu, Mingya Tan, Xiaojuan Deng and Zhenghuan Zhao
{"title":"Zinc–manganese sulfide nanoplatform for tumor-microenvironment-responsive chemodynamic/gas therapy and immunomodulation","authors":"Taotao Chu, Mengke Fan, Yu Guo, Meiling Liu, Mingya Tan, Xiaojuan Deng and Zhenghuan Zhao","doi":"10.1039/D5QM00815H","DOIUrl":"https://doi.org/10.1039/D5QM00815H","url":null,"abstract":"<p >Chemodynamic therapy (CDT) holds promise for cancer treatment, yet its efficacy is often limited by insufficient hydrogen peroxide (H<small><sub>2</sub></small>O<small><sub>2</sub></small>) supply and the dense extracellular matrix (ECM) in solid tumors. To address these challenges, we developed polyethylene glycol-modified zinc–manganese sulfide nanoparticles (ZMSPN) that integrate CDT, gas therapy, and tumor microenvironment modulation within a single pH-responsive platform. Upon reaching the acidic tumor microenvironment, ZMSPN simultaneously release zinc ions (Zn<small><sup>2+</sup></small>), manganese ions (Mn<small><sup>2+</sup></small>), and hydrogen sulfide (H<small><sub>2</sub></small>S). The released Mn<small><sup>2+</sup></small> ions generate cytotoxic hydroxyl radicals (˙OH) <em>via</em> a Fenton-like reaction, while H<small><sub>2</sub></small>S amplifies this effect by inhibiting catalase (CAT) to preserve endogenous H<small><sub>2</sub></small>O<small><sub>2</sub></small>. Meanwhile, Zn<small><sup>2+</sup></small> ions upregulate matrix metalloproteinase-2 (MMP-2) expression, promoting collagen degradation and enhancing drug penetration. Notably, this coordinated release creates a self-amplifying therapeutic cascade with H<small><sub>2</sub></small>S-enhanced CDT combined with Zn<small><sup>2+</sup></small> ion-mediated ECM remodeling that distinguishes ZMSPN from conventional platforms. Beyond direct tumor cell killing, ZMSPN treatment induces immunogenic modulation, as evidenced by damage-associated molecular patterns (DAMPs) and enhanced intratumoral T cell infiltration, indicating favorable remodeling of the tumor immune microenvironment. Additionally, the responsive release of Mn<small><sup>2+</sup></small> ions enables T<small><sub>1</sub></small>-weighted magnetic resonance imaging (MRI) for real-time treatment monitoring. By integrating these synergistic mechanisms, ZMSPN achieve potent antitumor efficacy with multifunctional capabilities in a single nanoplatform.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 11","pages":" 1850-1861"},"PeriodicalIF":6.4,"publicationDate":"2026-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148104184","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}
Su-Yun Zhang, Zhu Ding, Zihao Wang, Junzhe Tao and Yu-Jia Zeng
{"title":"Tunable exchange bias in Hofmann MOF-derived α-Fe2O3/Pt magnetic composites","authors":"Su-Yun Zhang, Zhu Ding, Zihao Wang, Junzhe Tao and Yu-Jia Zeng","doi":"10.1039/D6QM00110F","DOIUrl":"https://doi.org/10.1039/D6QM00110F","url":null,"abstract":"<p >The pursuit of strong, tunable, and thermally robust exchange bias (EB) is not only a fundamental scientific challenge but also a critical prerequisite for advancing spintronic technologies. Bottom-up designed nanostructures offer a versatile platform for engineering EB, owing to their precise control over composition, morphology, and assembly. However, studies on the EB effect in MOF-derived magnetic nanocomposites remain less unexplored. This study reports the EB effect in α-Fe<small><sub>2</sub></small>O<small><sub>3</sub></small>/Pt composites obtained <em>via</em> the pyrolysis of Hofmann-like Pt/Fe MOF at 450 °C, 550 °C, and 650 °C. The results show that Pt particles are dispersed on the α-Fe<small><sub>2</sub></small>O<small><sub>3</sub></small> particles, forming α-Fe<small><sub>2</sub></small>O<small><sub>3</sub></small>/Pt composites. The magnetic properties of samples are characterized by zero-field-cooled (ZFC) and field-cooled (FC) susceptibility as well as hysteresis loop measurements. Notably, a significant EB effect is observed in all samples and the optimized sample pyrolyzed at 450 °C exhibits the largest <em>H</em><small><sub>EB</sub></small> of 2099 Oe at 2 K under a cooling field of 40 kOe, which exceeds that of pure α-Fe<small><sub>2</sub></small>O<small><sub>3</sub></small> and other α-Fe<small><sub>2</sub></small>O<small><sub>3</sub></small> based composites. These findings highlight the calcination temperature as a critical parameter for tailoring the EB effect in MOF-derived oxide/metal nanocomposites.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 11","pages":" 1803-1812"},"PeriodicalIF":6.4,"publicationDate":"2026-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148104181","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}
Qian Zhang, Lin Ma, Guowei Wang, Yuhang Huang, Luyang Du, Taifeng Lin and Zhengguang Yan
{"title":"Tb-doped MA0.89FA0.11PbBr3 perovskite single crystals for gamma-ray detection","authors":"Qian Zhang, Lin Ma, Guowei Wang, Yuhang Huang, Luyang Du, Taifeng Lin and Zhengguang Yan","doi":"10.1039/D6QM00058D","DOIUrl":"https://doi.org/10.1039/D6QM00058D","url":null,"abstract":"<p >Rare-earth doping has emerged as a promising strategy to tailor the optoelectronic properties of metal halide perovskites, yet its potential for enhancing gamma-ray detection performance remains underexplored. The synthesis of large-sized, rare-earth doped perovskite single crystals remains challenging due to the adverse effects of dopants on crystal growth and lattice stability. Herein, we achieved 16 mm sized MA<small><sub>0.89</sub></small>FA<small><sub>0.11</sub></small>PbBr<small><sub>3</sub></small>:Tb single crystals (Tb/Pb = 0.13–0.67%) <em>via</em> nucleation control and precursor regulation. The X-ray fluorescence mapping confirms the uniform distribution of Tb<small><sup>3+</sup></small> within the crystal lattice at a low Tb/Pb ratio (≤0.35%). The successful incorporation of rare earth ions and a concomitant lattice contraction profoundly enhance the charge transport characteristics. Specifically, doping with 0.13% Tb<small><sup>3+</sup></small> increased the carrier mobility from 55 to 154 cm<small><sup>2</sup></small> V<small><sup>−1</sup></small> s<small><sup>−1</sup></small> and prolonged the carrier lifetime from 197 to 4422 ns. Consequently, the fabricated gamma-ray detector achieved a high energy resolution of 4.3% for <small><sup>241</sup></small>Am radiation (59.5 keV), a significant improvement over 15.7%. This work demonstrates rare-earth doping as an effective strategy toward high-performance perovskite radiation sensors.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 10","pages":" 1705-1712"},"PeriodicalIF":6.4,"publicationDate":"2026-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147958944","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":"One-pot synthesis of a quaternary ammonium-functionalized methylene blue-backboned polymer for robust NADH oxidation","authors":"Xuetong Cai, Chi Meng, Yajie Zhang and Fude Feng","doi":"10.1039/D5QM00778J","DOIUrl":"10.1039/D5QM00778J","url":null,"abstract":"<p >Compared to natural oxidases, artificial NADH oxidase (NOX) has distinct advantages in terms of cost, stability and manufacturing. Methylene blue is a redox-active phenothiazine derivative with a weak NOX-like activity in mediating electron transfer. Herein, we used a one-pot iron-catalyzed oxidative polymerization method to prepare a methylene blue-backboned polymer (MBPN-10) with pendant quaternary ammonium groups and compared its catalytic activity for NADH oxidation with that of methylene blue. MBPN-10 showed increased NADH binding affinity, improved catalytic performance, and increased shelf-life and was compatible with organic solvents. The reaction catalyzed by MBPN-10 is efficient and affords H<small><sub>2</sub></small>O<small><sub>2</sub></small> without the need for metals or light. These features make MBPN-10 a highly promising synthetic NOX mimic.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 11","pages":" 1813-1820"},"PeriodicalIF":6.4,"publicationDate":"2026-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147879455","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}
Mona Alshammari, Asma Alajmi, Bashayr Alanazi, Alotaibi Hanadi, Adel Alrehaili, Alaa Al-Jobory, Colin Lambert and Ali Ismael
{"title":"Tuning macrocyclic thermoelectrics via thiophene regioisomerism","authors":"Mona Alshammari, Asma Alajmi, Bashayr Alanazi, Alotaibi Hanadi, Adel Alrehaili, Alaa Al-Jobory, Colin Lambert and Ali Ismael","doi":"10.1039/D5QM00845J","DOIUrl":"https://doi.org/10.1039/D5QM00845J","url":null,"abstract":"<p >Quantum interference (QI) in single-molecule junctions exhibits robust effects at room temperature, which can be intuitively modeled using quantum circuit rules (QCR) and magic ratio (MR) theory. These frameworks describe how molecular conductance is governed by constituent moieties and their connectivity. Here, we apply these principles to explore the thermoelectric properties of a series of macrocyclic structures featuring multiple electron pathways, with mixed <em>meta</em> and <em>para</em> connectivities. Our density functional theory (DFT) calculations rationalize the experimentally measured conductance trends, demonstrating excellent agreement between theory and experiment. Furthermore, we predict that these macrocyclic junctions achieve significantly higher Seebeck coefficients than conventional single-branched analogues. A key finding is that strategic repositioning of sulfur atoms within the thiophene rings enables fine tuning of QI, modulating conductance and thermoelectric performance. Our work establishes macrocyclic architectures with tunable connectivities as a highly promising platform for advanced molecular thermoelectrics.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 9","pages":" 1510-1518"},"PeriodicalIF":6.4,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/qm/d5qm00845j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Guoye Yu, Ruoxuan Zhang, Xin Zhao, Jiaojiao Bi, Guangchao Han, Yingjie Zhao and Yuancheng Wang
{"title":"Structural regulation of covalent organic frameworks via isomerism for enhanced photocatalytic hydrogen peroxide production","authors":"Guoye Yu, Ruoxuan Zhang, Xin Zhao, Jiaojiao Bi, Guangchao Han, Yingjie Zhao and Yuancheng Wang","doi":"10.1039/D6QM00052E","DOIUrl":"https://doi.org/10.1039/D6QM00052E","url":null,"abstract":"<p >Covalent organic frameworks (COFs) have emerged as promising photocatalysts due to their well-defined porous structures and structural versatility. Among various design strategies, isomerism offers an efficient yet underexplored approach to modulating the structural and electronic properties of COFs without altering their chemical compositions. In this work, two regioisomeric COFs were rationally synthesized from isomeric cyano-substituted distyrylnaphthalene-based monomers to systematically investigate the effect of regioisomerism on photocatalytic behavior. Despite their identical chemical compositions, the two COFs exhibit distinct pore structures and markedly different photocatalytic performance. Notably, the <em>trans</em>-COF exhibited a significantly higher H<small><sub>2</sub></small>O<small><sub>2</sub></small> production rate of 3.34 mmol g<small><sup>−1</sup></small> h<small><sup>−1</sup></small> using 10% benzyl alcohol as a sacrificial agent, approximately three times higher than that of the <em>cis</em>-COF. Combined experimental and theoretical studies revealed that regioisomerism critically modulates the optoelectronic properties and charge-transfer characteristics of COFs, thereby governing their photocatalytic activity. This work provides new insights into the molecular-level rational design of efficient COF-based photocatalysts.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 10","pages":" 1683-1690"},"PeriodicalIF":6.4,"publicationDate":"2026-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147958942","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":"Mechanistic insights into PFOS and PFOA adsorption on acid-resistant MgTiO3","authors":"Seulgee Lee, Fumitaka Hayashi, Kunio Yubuta, Eugenio Otal, Nagahiro Saito, Hideki Tanaka and Katsuya Teshima","doi":"10.1039/D6QM00105J","DOIUrl":"https://doi.org/10.1039/D6QM00105J","url":null,"abstract":"<p >This study explores magnesium titanate (MgTiO<small><sub>3</sub></small>; MTO) as a durable ceramic adsorbent for per- and polyfluoroalkyl substance (PFAS) remediation under extreme acidic conditions. MTO exhibits outstanding acid resistance, retaining its crystal structure even at pH 1.0 with negligible Mg and Ti leaching. At pH 4.5, adsorption isotherms reach saturation, yielding maximum capacities of 8.92 mg g<small><sup>−1</sup></small> for perfluorooctane sulfonate (PFOS) and 6.42 mg g<small><sup>−1</sup></small> for perfluorooctanoic acid (PFOA). Adsorption kinetics show rapid uptake, followed by a slower diffusion-controlled regime, with apparent equilibration times of ∼120 min for PFOS and ∼300 min for PFOA. Time-resolved kinetic analyses, including square-root-of-time, pseudo-second-order, and double-exponential models, reveal a characteristic two-stage adsorption process dominated by diffusion resistance. Two-site Langmuir isotherms further support this behaviour by distinguishing high-affinity and non-specific adsorption domains. Spectroscopic analyses elucidate distinct adsorption mechanisms: PFOS adsorbs predominantly <em>via</em> an outer-sphere electrostatic pathway constrained by surface crowding, whereas PFOA undergoes a transition from site-specific inner-sphere coordination at Mg/Ti sites to slower outer-sphere accumulation. These findings demonstrate that PFOS and PFOA exhibit fundamentally different adsorption mechanisms on the same ceramic surface, governed by headgroup chemistry and surface coordination. By integrating exceptional acid durability with mechanistic insight, this work provides a foundation for the rational design of PFAS adsorbents for aggressive industrial wastewater treatment.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 9","pages":" 1461-1472"},"PeriodicalIF":6.4,"publicationDate":"2026-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808131","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}
Yitian Pan, Derong Cao, Xueguang Ran and Lingyun Wang
{"title":"Boosting photothermal conversion through a simultaneous donor engineering and boron complexation strategy for solar-driven applications","authors":"Yitian Pan, Derong Cao, Xueguang Ran and Lingyun Wang","doi":"10.1039/D5QM00898K","DOIUrl":"https://doi.org/10.1039/D5QM00898K","url":null,"abstract":"<p >Organic photothermal materials facilitate the direct conversion of solar energy into thermal energy <em>via</em> a method that is safe and adaptable and generates no pollution. However, their limitations, including narrow absorption spectra, low molar absorption coefficients in the NIR region, and insufficient nonradiative decay, impair the photothermal conversion efficiency (PCE) and hamper their potential applications. Herein, we present an effective strategy, “simultaneous donor engineering and boron complexation”, to enhance the photothermal conversion capability. Specifically, following the optimization of the donor from phenyl- to thienyl- and to triphenyl-amine (TPA) and modulating the aggregated architecture through boron complexation, six donor–acceptor-type molecules (<strong>Ph-H</strong>, <strong>Ph-BF<small><sub>2</sub></small></strong>, <strong>Th-H</strong>, <strong>Th-BF<small><sub>2</sub></small></strong>, <strong>TPA-H</strong> and <strong>TPA-BF<small><sub>2</sub></small></strong>) were designed and synthesized. The single-crystal structures of <strong>TPA-H</strong> and <strong>TPA-BF<small><sub>2</sub></small></strong> unveiled the regulatory effect of the coordination structure on their aggregates and packing modes. The loose and zigzag arrangement of the <strong>TPA-H</strong> dimers turned into the tight molecular packing of the <strong>TPA-BF<small><sub>2</sub></small></strong> dimers, facilitating an improvement in PCE by simultaneously broadening their absorption spectra, increasing their molar absorption coefficients in the UV-vis-NIR region, and enhancing nonradiative decay. It is demonstrated that the PCE can be effectively tuned from 8.4% (<strong>Ph-BF<small><sub>2</sub></small></strong>) to 26.4% (<strong>TPA-BF<small><sub>2</sub></small></strong>). As a consequence, under 1 sun (1.0 kW m<small><sup>−2</sup></small>) exposure, the water evaporation rate, solar-to-vapor efficiency and voltage output of <strong>TPA-BF<small><sub>2</sub></small></strong> improved by 1.43, 1.44, and 1.45 times those of <strong>Ph-BF<small><sub>2</sub></small></strong>, respectively. Among them, <strong>TPA-BF<small><sub>2</sub></small></strong> exhibited an outstanding water evaporation rate of 1.321 kg m<small><sup>−2</sup></small> h<small><sup>−1</sup></small>, a high solar-to-vapor efficiency of 90.5%, and a high voltage output (198 mV) in a solar thermoelectric generator under 1 sun irradiation. The practical purification ability of seawater was also investigated. This study provides guidelines for the rational design of high-performance organic photothermal materials.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 10","pages":" 1644-1659"},"PeriodicalIF":6.4,"publicationDate":"2026-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147958920","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}
Qilong Liu, Cheng Gong, Xiaole Zhang, Peng Chen, Mengxiang Wang, Qizhu Qian, Jujia Zhang, Mingliang Fang and Wentuan Bi
{"title":"Template-assisted synthesis of amorphous NiFeCuOx arrays for efficient anion-exchange membrane water oxidation","authors":"Qilong Liu, Cheng Gong, Xiaole Zhang, Peng Chen, Mengxiang Wang, Qizhu Qian, Jujia Zhang, Mingliang Fang and Wentuan Bi","doi":"10.1039/D6QM00077K","DOIUrl":"https://doi.org/10.1039/D6QM00077K","url":null,"abstract":"<p >Hydrogen production <em>via</em> an anion-exchange membrane (AEM) water electrolyzer has emerged as one of the most promising strategies for large-scale hydrogen generation, owing to its low cost, rapid response, and modular scalability. However, the oxygen evolution reaction (OER) at the anode still suffers from intrinsically sluggish four-electron-transfer kinetics, which remains a critical bottleneck to commercialization. In this work, we synthesized an amorphous NiFe-based hierarchical array OER catalyst using a template-assisted method. This hierarchical array promotes rapid electron transport and exposes abundant active sites, exhibiting an overpotential of 283 mV to achieve a current density of 100 mA cm<small><sup>−2</sup></small> and stable operation for more than 100 h. Furthermore, <em>in situ</em> electrochemical Raman spectroscopy revealed the structural transformation of Ni active sites during the OER. The AEM water electrolyzer assembled with the NiFeCuO<small><sub><em>x</em></sub></small> array catalysts delivers an industrial-level current density of 2.7 A cm<small><sup>−2</sup></small> at 2.0 V<small><sub>cell</sub></small>. This template-assisted synthesis method provides a new pathway for constructing NiFe-based OER catalysts and also offers valuable insights for advancing the commercial implementation of AEM electrolysis technology.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 10","pages":" 1668-1674"},"PeriodicalIF":6.4,"publicationDate":"2026-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147958922","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}
Shubing Li, Tianyu Xia, Yuxin Zhao, Lingrui Wang, Fan Meng, Noriyoshi Arai, Haizhong Guo and Rongming Wang
{"title":"Ni–OH promoted water dissociation on Pt/Ni dual active sites for accelerated alkaline hydrogen evolution","authors":"Shubing Li, Tianyu Xia, Yuxin Zhao, Lingrui Wang, Fan Meng, Noriyoshi Arai, Haizhong Guo and Rongming Wang","doi":"10.1039/D6QM00002A","DOIUrl":"https://doi.org/10.1039/D6QM00002A","url":null,"abstract":"<p >Although Pt–M (M = transition metal) catalysts are indispensable for the hydrogen evolution reaction (HER), the key function and operative mechanism of M that extend beyond the electronic modulation of Pt remain poorly defined. To address this gap, we synthesized three-dimensional PtNi multibranched nanostructures (PtNi MBNs) incorporating dual active sites. <em>In situ</em> spectroscopic analyses reveal that Ni sites directly facilitate water dissociation through the generation of Ni–OH species, thereby producing ample H* intermediates that mitigate the hydrogen scarcity in alkaline electrolytes and subsequently enhance the formation of Pt–H bonds. Molecular dynamics simulations further confirm strong spontaneous bonding between Ni and O at the atomic scale, underscoring the critical role of Ni in driving water dissociation and stabilizing Ni–OH bonds. Such Pt/Ni dual-active-site mechanism endows the PtNi MBNs with exceptional performance in 1 M KOH, delivering an ultralow overpotential of 9.29 mV at 10 mA cm<small><sup>−2</sup></small> (35.2 mV lower than Pt/C) and a high mass activity of 9.30 A mg<small><sub>Pt</sub></small><small><sup>−1</sup></small> at −70 mV (3.63 times that of Pt/C). Characterization after cycling confirmed that PtNi MBNs exhibit excellent structural stability and electrochemical stability. This study advances the fundamental understanding beyond single site catalytic mechanisms and offers new insights for accelerating HER kinetics in alkaline electrolytes.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 9","pages":" 1487-1496"},"PeriodicalIF":6.4,"publicationDate":"2026-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808133","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}