Pedro Y. S. Nakasu*, , , Maite A. Martinez, , , Susiana Melanie, , , Talia A. Shmool, , and , Jason P. Hallett,
{"title":"Correction to “Chitosan-Based Biocomposite Hydrogels with Squid Pen Protein for Anionic Dyes Adsorption”","authors":"Pedro Y. S. Nakasu*, , , Maite A. Martinez, , , Susiana Melanie, , , Talia A. Shmool, , and , Jason P. Hallett, ","doi":"10.1021/acsmaterialslett.5c00937","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00937","url":null,"abstract":"<p >Growing environmental concerns have driven the search for sustainable wastewater treatment solutions, particularly for removing persistent synthetic dyes. This study explores hydrogels made from squid pen protein (SPP) and chitosan, biodegradable polymers, for anionic dye adsorption─reactive blue 4 (RB4) and methyl orange (MO). A 50%/50% SPP/chitosan hydrogel was optimal for RB4 adsorption while minimizing chitosan use. Adsorption followed the Langmuir model, with capacities of 151.52 mg/g for RB4 and 54.94 mg/g for MO. Optimal RB4 adsorption conditions were 65 °C, 6 h, pH 7, and 0.2 wt % adsorbent at 300 rpm. Kinetic analysis indicated a pseudo-second-order model, suggesting chemisorption. Characterization (FT-IR, SEM, XPS) revealed functional groups and binding mechanisms, with XPS confirming a nucleophilic attack between the amino groups of chitosan/SPP protein and RB4’s dichlorotriazine moiety. Higher cross-linker content reduced adsorption. This study demonstrates SPP/chitosan hydrogels as a cost-effective, sustainable alternative for wastewater treatment.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3291"},"PeriodicalIF":8.7,"publicationDate":"2025-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00937","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226783","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Toward Anode-less Lithium Metal Batteries Enabled by Garnet-Based Composite Polymer Electrolytes","authors":"Pavitra Srivastava, , , Yuan-Ting Hung, , , Chih-Yang Cheng, , , Shun-Ming Huang, , , Yi-Tso Wu, , and , Ru-Shi Liu*, ","doi":"10.1021/acsmaterialslett.5c00838","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00838","url":null,"abstract":"<p >A promising strategy for next-generation energy storage involves boosting the energy density through innovative cell architectures. Among these architectures, anode-less Li metal batteries stand out for their potential to eliminate excess Li, thus maximizing energy density and simplifying manufacturing. Most anode-less systems rely on liquid or inorganic solid electrolytes, each with safety and scalability limitations. This work demonstrates the feasibility of an anode-less system enabled by garnet-based composite polymer electrolytes with high ionic conductivity (∼1.4 mS cm<sup>–1</sup> at 50 °C). A Cu–In current collector on the anode side was optimized to promote uniform Li nucleation and alloy formation. Full cells exhibited stable cycling for 200 cycles, with an average Coulombic efficiency of 96.2%. Although this work did not target high capacity, it provides a crucial proof of concept, highlighting the practical viability of a polymer-based anode-less Li metal battery for future high-energy-density battery systems.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3283–3290"},"PeriodicalIF":8.7,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00838","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226775","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Solvent-Mediated Electrolyte Design for Calcium Metal Batteries","authors":"Zaher Slim*, , , Carolina Cruz-Cardona, , , Clément Pechberty, , , Tomooki Hosaka, , , Zoran Mandić, , , Vladimir Panic, , and , Patrik Johansson, ","doi":"10.1021/acsmaterialslett.5c00892","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00892","url":null,"abstract":"<p >Current electrolytes for calcium batteries (CaBs) rely on cumbersome salt synthesis, hindering research and development. As a subclass of CaBs, calcium metal batteries (CMBs) could potentially offer high energy density due to their use of a calcium anode. However, realizing this advantage remains difficult, largely due to calcium’s electrochemical instability. To address these challenges, we introduce a family of electrolytes made entirely from commercially accessible Ca-salts and solvent mixtures and further demonstrate stable cycling of symmetric Ca||Ca cells using only a solvent mixture, without added salt (i.e., not being an electrolyte on its own). Notably, this cycling stability extends to CMB full cells using low salt concentration electrolytes (e.g., 0.1 M Ca(OTf)<sub>2</sub> in NMA:TMP), and similar full cell performance is also achieved using other combinations of salts and solvent mixtures. Extensive electrochemical testing confirms stable cycling under diverse and challenging conditions. Overall, our findings reframe electrolyte design principles and pave the way for practically useful CMB cells.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3235–3242"},"PeriodicalIF":8.7,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00892","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226774","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Metal–Organic Frameworks for Per- and Polyfluoroalkyl Substances Treatment in Contaminated Water","authors":"Rong-Ran Liang, , , Zhaoyi Liu, , , Joshua Rushlow, , , Jiatong Huo, , , Zongsu Han, , , Yihao Yang, , , Hengyu Lin, , and , Hong-Cai Zhou*, ","doi":"10.1021/acsmaterialslett.5c00902","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00902","url":null,"abstract":"<p >Per- and polyfluoroalkyl substances (PFAS) are synthetic pollutants known for their chemical stability, environmental persistence, and toxicological risks. Their widespread use has led to extensive contamination, particularly in aquatic systems. Conventional treatment methods often face challenges such as high energy consumption and the production of secondary pollutants. Metal–organic frameworks (MOFs), with their high surface areas and tunable structures, have emerged as promising materials for PFAS remediation. This review summarizes recent progress in MOF-based PFAS adsorption and degradation, highlighting key frameworks such as MIL, UiO, and ZIF. Mechanistic insights into adsorption behavior and regeneration capabilities are discussed, along with the catalytic performance of MOF composites and postmodified systems in degradation pathways. The review concludes with design strategies for next-generation MOF materials aimed at efficient, sustainable PFAS removal under realistic conditions.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3252–3274"},"PeriodicalIF":8.7,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00902","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226811","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Muhammad Faisal Anwar, , , Muhammad Afzal, , , Muhammad Khalid, , , Muhammad Imran Asghar, , , Liangdong Fan, , , Sining Yun, , , Touseef Ahmad, , , Li Sun, , , Peter D Lund*, , and , Bin Zhu*,
{"title":"Proton Conduction in Oxides Via Electrochemical Proton Injection and Proton–Electron Spillover","authors":"Muhammad Faisal Anwar, , , Muhammad Afzal, , , Muhammad Khalid, , , Muhammad Imran Asghar, , , Liangdong Fan, , , Sining Yun, , , Touseef Ahmad, , , Li Sun, , , Peter D Lund*, , and , Bin Zhu*, ","doi":"10.1021/acsmaterialslett.5c00855","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00855","url":null,"abstract":"<p >Proton conduction in oxides (PCOs) is traditionally explained by hydration-based equilibrium models, which assume sufficient proton uptake from moisture or hydrogen. However, this static hydration-based framework fails under real operating conditions of proton ceramic fuel cells, where proton injection and field-driven dynamic processes dominate. This disconnection has led to an underestimation of proton concentration and mobility, also limiting the development of advanced PCOs. Here, we establish a distinct fundamental and experimental framework based on electrochemical proton injection (EPI) and proton–electron spillover, which are dynamic processes enabling an enhanced proton transport both in bulk and across grain boundary domains. Supported by in situ electrochemical impedance spectroscopy and the distribution of relaxation time, we demonstrate that EPI surpasses the conductivity ceiling imposed by the hydration-limited models. This urgent correction restores the true basis of proton transport and suggests a transformative strategy for designing next-generation oxide electrolytes for electrochemical energy devices.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3275–3282"},"PeriodicalIF":8.7,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226812","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}
{"title":"Discrimination of Single and Isomeric Amino Acids in Peptides Using a Multi-Walled Carbon Nanotube Porin Sensing System","authors":"Junzhou He, , , Gensheng Wu, , and , Wei Si*, ","doi":"10.1021/acsmaterialslett.5c00676","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00676","url":null,"abstract":"<p >Precise amino acid identification is critical for many biological applications but remains limited by the lack of methods to resolve subtle differences between proteinogenic residues and their substitutions. Here, we present a multi-walled carbon nanotube porin sensing system to identify single and isomeric amino acids in peptides. Molecular dynamics simulations reveal that strong van der Waals (vdW) interactions between peptide side chains and the nanotube interior slow translocation, with the interaction strength varying by amino acid. By utilizing the smooth tubular structure of the carbon nanotube’s inner wall, we demonstrate the ability to simultaneously consider steric hindrance effects and vdW interactions as the primary factors for distinguishing proteinogenic amino acids. We show that the sensing system can directly identify up to 10 proteinogenic amino acids, including isomers, and locate single-residue substitutions in peptides at subnanometer resolution. These findings have the potential to lay the foundation for protein sequencing.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3243–3251"},"PeriodicalIF":8.7,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226810","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}
{"title":"Ultraflexible Organic Room-Temperature Phosphorescent Crystals","authors":"Jingyu Cao, , , Jinming Song*, , , Ying Hu, , , Fengling Zhang, , , He Tian, , and , Xiang Ma*, ","doi":"10.1021/acsmaterialslett.5c01042","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01042","url":null,"abstract":"<p >Flexible organic room-temperature phosphorescence (RTP) crystals have attracted attention in optoelectronic materials due to their unique mechanical advantages. Herein we report a bottom-up strategy to realize both ultraflexibility and pure RTP emission through multiple-hydrogen-bond self-assembly. Specifically, the quadruple carbonyl group of the substituted 1,4-bis(phenylglyoxalyl)benzene (DBs) molecule not only performs as a hydrogen-bond acceptor to direct the flexible assembly but also provides strong intersystem crossing effects to realize pure RTP emission. By modulation of substituted aromatic groups, mechanical tunability from brittle to ultraflexible (ε<sub>max</sub> = 6.76%) can be achieved in DBs crystals. Furthermore, pure RTP emission (including near-infrared) is realized, which is a virtually unexplored area of flexible crystals. Binding energy calculations further confirm the flexible assembly mechanism of multiple hydrogen bonds. Overall, the reported crystal assemblies demonstrate impressive mechanical elastic flexibility and pure RTP emission, providing a supramolecular approach for the design of ultraflexible photoelectric crystals.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3227–3234"},"PeriodicalIF":8.7,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226789","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}
{"title":"Two-Dimensionality and Electron Doping Enhance Superconductivity in a SnSe2–Co(Cp)2 Organic–Inorganic Hybrid Superlattice","authors":"Yuliang Li, , , Yingcheng Zhao, , , Zejun Li, , , Kejun Mu, , , Chengcheng Ao, , , Tongrui Li, , , Zhanfeng Liu, , , Shengtao Cui, , , Lidong Zhang, , , Guobin Zhang, , , Yuqiao Guo, , , Zhe Sun*, , , Changzheng Wu*, , and , Yi Liu*, ","doi":"10.1021/acsmaterialslett.5c00951","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00951","url":null,"abstract":"<p >The tunability of transition metal dichalcogenides (TMDs) makes them ideal platforms for exploring emergent phenomena. While superconductivity has been observed in 1T-SnSe<sub>2</sub> intercalated with cobaltocene Co(Cp)<sub>2</sub>, the underlying electronic mechanisms remain unclear. Using angle-resolved photoemission spectroscopy (ARPES), we investigate the electronic structure evolution from pristine 1T-SnSe<sub>2</sub> to the SnSe<sub>2</sub>–Co(Cp)<sub>2</sub> superlattice. We observe increased two-dimensionality in the superlattice and electron doping of the SnSe<sub>2</sub> conduction band minimum. This dimensional change, combined with the higher charge carrier density, significantly increases the density of states near the Fermi level, a key factor for superconductivity. Our findings demonstrate the effectiveness of organic molecular intercalation for manipulating electronic dimensionality and inducing superconductivity in TMD-based heterostructures.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3213–3219"},"PeriodicalIF":8.7,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226788","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}
{"title":"Toward Circularly Polarized Luminescence from Inherently Chiral Inverted Singlet–Triplet Chromophores","authors":"Simone Veglianti, , , Alessandro Michieletti, , and , Daniele Padula*, ","doi":"10.1021/acsmaterialslett.5c00872","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00872","url":null,"abstract":"<p >Recent years have seen rising interest in molecules that violate Hund’s rule, where the first excited singlet state lies below the triplet (Δ<i>E</i><sub><i>ST</i></sub> < 0), accelerating reverse intersystem crossing, a key process in thermally activated delayed fluorescence. We present a computational study on such inverted singlet–triplet (IST) molecules modified for chirality to enable Circularly Polarized Luminescence (CPL), an unexplored direction for IST emitters. Two main chromophores, triangulene and pentalene, were functionalized with minimal chiral groups, preserving negative Δ<i>E</i><sub><i>ST</i></sub>, as demonstrated via multiconfigurational calculations. We also explored inherently chiral, nonplanar chromophores, focusing on extended triangulenes resembling helicenes. Substituents enabling enantiomer separation were introduced, and racemization barriers were assessed. When singlet–triplet inversion was lost, structures were further optimized, yielding a promising substrate combining a high racemization barrier, strong CPL, and inverted singlet–triplet energetics, making it suitable for CP-OLED applications.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 10","pages":"3220–3226"},"PeriodicalIF":8.7,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00872","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145226787","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sabrina J. Curley, and , Caroline R. Szczepanski*,
{"title":"Applying Hansen Solubility Parameters to Dynamically Reacting Systems─A Case Study of Photopolymerization Induced Phase Separation","authors":"Sabrina J. Curley, and , Caroline R. Szczepanski*, ","doi":"10.1021/acsmaterialslett.5c00598","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00598","url":null,"abstract":"<p >Photopolymerization induced phase separation (PIPS) is a straightforward strategy for complex design, where homogeneous starting resins form chemically heterogeneous materials, overcoming limitations of traditional patterning approaches. To minimize resource waste when exploring undiscovered PIPS systems and applications, it is necessary to identify prediction and screening tools that appropriately eliminate nonviable resin combinations. Here we use Hansen Solubility Parameters (HSPs) as a screening strategy to predict solubility interactions of PIPS resin components at the initial and final stages of a reaction. With these two states in mind, the degrees of miscibility between available precursors (e.g., (co)monomers and polymer additives) can be leveraged to identify promising PIPS resin systems. We demonstrate that in using solubility parameters to inform PIPS resin design, HSPs can streamline resin formulation and exploration. We implemented this approach to create photopolymers with engineered wettability gradients.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 9","pages":"3206–3212"},"PeriodicalIF":8.7,"publicationDate":"2025-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00598","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144921004","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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