ChemPub Date : 2026-04-27DOI: 10.1016/j.chempr.2026.103032
Kanglei Pang, Chang Long, Jiayin Yuan
{"title":"Operando X-ray spectroscopies for tracking electrocatalytic dynamic interfaces across multiple scales","authors":"Kanglei Pang, Chang Long, Jiayin Yuan","doi":"10.1016/j.chempr.2026.103032","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103032","url":null,"abstract":"The catalyst-electrolyte interface (CEI) fundamentally plays a vital role in governing the activity and kinetics of electrochemical reactions relevant to chemical manufacturing, energy devices, and other applications. However, state-of-the-art observations of the CEI reveal structural evolution during reactions, leading to challenges in elucidating the true structure-performance relationships and thereby hindering the rational design of high-performance catalytic systems for emerging applications. This perspective highlights advances in <ce:italic>operando</ce:italic> X-ray spectroscopies that enable a mechanistic understanding of dynamic CEI across electronic-, atomic-, and nanoscale levels. We highlight the challenges and opportunities regarding X-ray spectroscopies for understanding, predictive design, and durability engineering of the CEI in heterogeneous electrocatalysis.","PeriodicalId":268,"journal":{"name":"Chem","volume":"21 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147752944","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}
ChemPub Date : 2026-04-21DOI: 10.1016/j.chempr.2026.103038
Hong Kang, Yuexuan Yang, Qishu Zhang, Qi Yan, Bryan Wei
{"title":"Polymerase-mediated expansion of DNA nanostructures","authors":"Hong Kang, Yuexuan Yang, Qishu Zhang, Qi Yan, Bryan Wei","doi":"10.1016/j.chempr.2026.103038","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103038","url":null,"abstract":"The development of DNA dynamics in synthetic constructs based on enzymatic treatment has lagged behind that of its rivals based on common strand displacement. In this work, we present an enzymatic expansion framework for DNA nanostructures. Using extendable loops positioned at the constituent edges to serve as templates for DNA polymerase-driven elongation, we have realized controllable unidirectional and multidirectional expansion. According to the scheme, enzymatic treatment results in controlled expansion up to ∼4-fold for two-dimensional and three-dimensional nanostructures. This high-performance dynamic control makes our method an attractive alternative to strand displacement techniques.","PeriodicalId":268,"journal":{"name":"Chem","volume":"24 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147726588","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":"Nanophase structuring in simple ternary solvents mediates reaction kinetics","authors":"Yifei Wang, Binish Ashfaq, Jung-Bin Ahn, Peiran Wei, Lauren D. Zarzar","doi":"10.1016/j.chempr.2026.103039","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103039","url":null,"abstract":"Solvents are crucial to chemical reactivity. Ternary mixtures of water, a water-miscible polar organic solvent, and a water-immiscible oil can self-organize into nanoscale domains (nanophases), yet their impact on reaction kinetics is not well understood. Here, we investigate how nanophase structuring affects strain-promoted azide-alkyne click (SPAAC) reaction kinetics. Ternary solvents were designed to promote or suppress nanophase structuring, characterized by dynamic light scattering (DLS) and small-angle X-ray scattering (SAXS). High-throughput ultraviolet-visible spectroscopy (UV-vis) kinetics revealed that hydrophobic reactants exhibited faster rates in ternary solvents compared with pure solvents and water-containing binary mixtures. Rate enhancements were confined to a narrow region of the phase diagram containing oil-in-water nanophases and disappeared when hydrophilic reactants were used or when nanophase stability was reduced. These findings demonstrate that simple ternary solvents modulate reaction kinetics in a manner distinct from bulk solvent polarity or conventional hydrophobic effects and highlight the potential of nanophases to control reactivity.","PeriodicalId":268,"journal":{"name":"Chem","volume":"224 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147709290","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}
ChemPub Date : 2026-04-17DOI: 10.1016/j.chempr.2026.103026
Fang-Zi Liu, Shi Li, Yufei Zhu, Yan Liu, Jian Wang, Heather J. Kulik, KaKing Yan
{"title":"Out-of-equilibrium confinement catalysis mediated by compressive force","authors":"Fang-Zi Liu, Shi Li, Yufei Zhu, Yan Liu, Jian Wang, Heather J. Kulik, KaKing Yan","doi":"10.1016/j.chempr.2026.103026","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103026","url":null,"abstract":"Biological systems sustain non-equilibrium states through continuous energy inputs such as light or chemical fuels, whereas synthetic systems typically dissipate energy toward equilibrium. Here, we demonstrate that mechanical force delivered via ball milling serves as a unique energy source to drive endergonic coordination self-assembly inaccessible through conventional stimuli. Mechanistic studies combining ball-milling kinetics, model reactions, and density functional theory (DFT) calculations reveal that direct mechanical impact strongly deforms coordination cages, elevating their ground-state energies. These distorted cages enable barrier-free guest release, followed by cage reassembly. By coupling this force-driven step with a subsequent equilibrium process, two unprecedented outcomes are achieved: (1) an out-of-equilibrium catalytic confinement cycle and (2) a dissipative cycle. Notably, this mechanochemical strategy circumvents product inhibition in equilibrium-based supramolecular systems, enabling transformations with up to 85 catalytic turnovers. Our work highlights mechanical force as a design principle for non-equilibrium chemistry toward life-like systems.","PeriodicalId":268,"journal":{"name":"Chem","volume":"19 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147709069","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}
ChemPub Date : 2026-04-17DOI: 10.1016/j.chempr.2026.103033
Yixin Li, Lin Yao, Jinglin Li, Tianqi Yu, Andreas Kafizas, Ying Li, Liang Qiu, Lam Jun Kay, Tao Wang, Md Afjalur Rahman, Nirmal Anand, Sharif Md. Sadaf, Baowen Zhou
{"title":"Water-triggered photocatalytic oxidative coupling of methane toward C2H6 over Au/GaN nanoarchitecture","authors":"Yixin Li, Lin Yao, Jinglin Li, Tianqi Yu, Andreas Kafizas, Ying Li, Liang Qiu, Lam Jun Kay, Tao Wang, Md Afjalur Rahman, Nirmal Anand, Sharif Md. Sadaf, Baowen Zhou","doi":"10.1016/j.chempr.2026.103033","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103033","url":null,"abstract":"Solar-driven oxidative coupling of methane (CH<sub>4</sub>) offers a sustainable route for synthesizing value-added chemicals beyond petroleum. To address current thermodynamic and selectivity challenges, a photocatalytic system employing nano-gold-decorated GaN nanowires is developed for the efficient conversion of CH<sub>4</sub> into ethane (C<sub>2</sub>H<sub>6</sub>), using water as a green oxidant. The optimized catalyst delivers a remarkable C<sub>2</sub>H<sub>6</sub> production rate of 112.6 mmol⋅g<sub>cat</sub><sup>−1</sup>⋅h<sup>−1</sup> with 94.9% selectivity and a turnover number of 40,824 after 256 h operation. Mechanistic investigations reveal that photogenerated holes trapped at Au sites oxidize H<sub>2</sub>O into highly active ·OH radicals. These radicals significantly lower the energy barrier for C<sub>2</sub>H<sub>6</sub> formation via an H-exchange mechanism. Ultimately, the synergistic Au/GaN interface inhibits CH<sub>4</sub> over-oxidation, showcasing a highly promising, environmentally friendly pathway for solar-to-chemical energy conversion.","PeriodicalId":268,"journal":{"name":"Chem","volume":"15 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147709250","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}
ChemPub Date : 2026-04-17DOI: 10.1016/j.chempr.2026.103036
Junhong Li, Martin Stroet, Vivian G. Shang, Wenrui Lyu, Jack K. Clegg, Evelyne Deplazes, Xin Wu
{"title":"Chasing nature’s anion binders","authors":"Junhong Li, Martin Stroet, Vivian G. Shang, Wenrui Lyu, Jack K. Clegg, Evelyne Deplazes, Xin Wu","doi":"10.1016/j.chempr.2026.103036","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103036","url":null,"abstract":"In water, hydrogen bonds between solute molecules are disfavored because they must compete with the overwhelming abundance of water forming hydrogen bonds with solutes. Thus, molecular recognition by hydrogen bonds in water has long been considered challenging, often requiring auxiliary interactions such as ion pairing and hydrophobic contacts. Yet through evolved structural sophistication, certain biological receptors such as sulfate-binding proteins use hydrogen bonds alone to bind hydrophilic anions with remarkable (sub)micromolar affinities. Here, we report highly pre-organized, uncharged hydrogen-bonding molecular cages that match the micromolar affinities of nature’s anion receptors in water. Contrasting large biological receptors that bury polar binding sites within hydrophobic cores, these synthetic hosts have just 52 heavy atoms with polar binding sites exposed to water. These results establish the capabilities of unshielded polar hydrogen bonds in aqueous supramolecular chemistry, providing new opportunities for biological interventions and molecular separations.","PeriodicalId":268,"journal":{"name":"Chem","volume":"47 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147709284","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}
ChemPub Date : 2026-04-17DOI: 10.1016/j.chempr.2026.103037
Evan L. Cline, Hyuk-Jun Noh, Georganna Benedetto, Gbenga Fabusola, Aiden Hawkins, Cory M. Simon, Katherine A. Mirica
{"title":"Array of bimetallic metallophthalocyanine-based metal-organic frameworks for chemiresistive detection and differentiation of toxic gases","authors":"Evan L. Cline, Hyuk-Jun Noh, Georganna Benedetto, Gbenga Fabusola, Aiden Hawkins, Cory M. Simon, Katherine A. Mirica","doi":"10.1016/j.chempr.2026.103037","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103037","url":null,"abstract":"Rapid, low-power, room-temperature gas sensors are essential for human health and safety. Conductive metal-organic frameworks (cMOFs), particularly bimetallic two-dimensional layered MOFs based on metallophthalocyanine (MPc), have emerged as modular chemiresistive materials capable of room-temperature and low-power operation with rapid responses to gaseous analytes. This paper describes the use of nine structurally analogous MPc-based cMOFs for the detection of toxic gases. When combined with both unsupervised and supervised machine learning algorithms to interpret the response pattern, this array achieves discrimination between H<sub>2</sub>S, NO, and CO analytes in N<sub>2</sub> at parts per million (ppm)-level concentrations. Spectroscopic studies and comparisons between the chemiresistive responses of the cMOFs revealed that their gaseous detection is dictated by the metal bis(dioxolene) moiety, which is involved in both gaseous analyte coordination and redox chemistry. This study opens the door to leveraging modular molecular design of reticular materials for strategic chemical detection in low-power, portable devices.","PeriodicalId":268,"journal":{"name":"Chem","volume":"22 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147726495","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":"The third wave of enzyme engineering: Navigating the AI-powered IDEA paradigm","authors":"Shuaiqi Meng, Shiwei Cheng, Xiao Cheng, Dongzhi Wei, Xiujuan Li, Haiyang Cui","doi":"10.1016/j.chempr.2026.103001","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103001","url":null,"abstract":"Enzyme engineering has evolved from random directed evolution to knowledge-guided rational design and is now entering an artificial intelligence (AI)-driven third wave. To capture AI’s transformative impact, we propose the investigate-design-execute-analyze (IDEA) framework, which illustrates how AI integrates across the entire enzyme engineering pipeline—from enzyme discovery and biocatalyst design to experimental validation and mechanistic analysis. This framework serves as a roadmap for leveraging advanced AI to reprogram enzyme engineering workflows, establishing a new paradigm for intelligent biocatalyst design.","PeriodicalId":268,"journal":{"name":"Chem","volume":"9 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147709282","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}
ChemPub Date : 2026-04-16DOI: 10.1016/j.chempr.2026.103030
Moon Hyeok Choi, Mike Filius, Senne Klomp, Yen Way Isabell Trinh, Adam Pomorski, Chirlmin Joo
{"title":"Single-molecule FRET enables the detection of site-specific α-synuclein serine phosphorylation","authors":"Moon Hyeok Choi, Mike Filius, Senne Klomp, Yen Way Isabell Trinh, Adam Pomorski, Chirlmin Joo","doi":"10.1016/j.chempr.2026.103030","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103030","url":null,"abstract":"Phosphorylation, a key posttranslational modification, plays a crucial role in regulating protein function and stability. However, conventional ensemble assays, such as ELISA, are unable to resolve phosphorylation at the proteoform level, thereby obscuring the heterogeneity of site-specific modifications. To address this limitation, we present a single-molecule analysis platform that combines site-specific labeling of phosphorylation sites with fluorescence resonance energy transfer (FRET) to pinpoint the location of phosphorylation sites in full-length proteins. We demonstrate the applicability of our approach on α-synuclein (αSyn), a protein implicated in neurodegenerative diseases. We can quantify the number of phosphorylation sites and identify which amino acids are phosphorylated on αSyn, depending on the type of kinase used. This single-molecule platform achieves picomolar (pM) sensitivity, enabling the detection of distinct phosphorylated proteoforms that are beyond the reach of conventional ensemble methods. Our approach enables detailed analysis of protein modifications in neurodegenerative diseases and may aid biomarker discovery.","PeriodicalId":268,"journal":{"name":"Chem","volume":"243 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147709280","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}
ChemPub Date : 2026-04-16DOI: 10.1016/j.chempr.2026.103061
Sha Bai, Ying-Feng Han
{"title":"Expanding the territory to post-assembly modification of metallacages","authors":"Sha Bai, Ying-Feng Han","doi":"10.1016/j.chempr.2026.103061","DOIUrl":"https://doi.org/10.1016/j.chempr.2026.103061","url":null,"abstract":"The functionalization of metallacages represents a pivotal prerequisite for unlocking their potential in biomedical applications. Now, Moreno-Alcántar, Casini, and co-workers report in <em>Cell Reports Physical Science</em> a comprehensive strategy enabling the efficient post-assembly modification (PAM) of Pt(II) cages via amide coupling and click chemistry for <em>in vivo</em> use. This strategy expands the scope of metallacage-based drug delivery, imaging, and supramolecular radiotheranostics.","PeriodicalId":268,"journal":{"name":"Chem","volume":"33 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2026-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147709281","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}