JACS Au最新文献

{"title":"Lipid-Directed Covalent Labeling of Plasma Membranes for Long-Term Imaging, Barcoding and Manipulation of Cells.","authors":"Nathan Aknine, Remi Pelletier, Andrey S Klymchenko","doi":"10.1021/jacsau.4c01134","DOIUrl":"10.1021/jacsau.4c01134","url":null,"abstract":"<p><p>Fluorescent probes for cell plasma membranes (PM) generally exploit a noncovalent labeling mechanism, which constitutes a fundamental limitation in multiple bioimaging applications. Here, we report a concept of lipid-directed covalent labeling of PM, which exploits transient binding to the lipid membrane surface generating a high local dye concentration, thus favoring covalent ligation to random proximal membrane proteins. This concept yielded fluorescent probes for PM called MemGraft, which are built of a dye (cyanine Cy3 or Cy5) bearing a low-affinity membrane anchor and a reactive group: an activated ester or a maleimide. In contrast to specially designed control dyes and commercial Cy3-based labels of amino or thiol groups, MemGraft probes stain efficiently PM, revealing the crucial role of the membrane anchor combined with optimal reactivity of the activated ester or the maleimide. MemGraft probes overcome existing limitations of noncovalent probes, which makes them compatible with cell fixation, permeabilization, trypsinization, and the presence of serum. The latter allows long-term cell tracking and video imaging of cell PM dynamics without the signs of phototoxicity. The covalent strategy also enables staining and long-term tracking of cocultured cells labeled in different colors without exchange of probes. Moreover, the combination of MemGraft-Cy3 and MemGraft-Cy5 probes at different ratios enabled long-term cell barcoding in at least 5 color codes, important for tracking and visualizing multiple populations of cells. Ultimately, we found that the MemGraft strategy enables efficient biotinylation of the cell surface, opening the path to cell surface engineering and cell manipulation.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"922-936"},"PeriodicalIF":8.5,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11863151/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143525721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Nanobiosensors Enable High-Efficiency Detection of Tuberculosis Nucleic Acid","authors":"Mei Li,&nbsp;Chen Shen,&nbsp;Min Lv* and Yao Luo*,&nbsp;","doi":"10.1021/jacsau.4c0120610.1021/jacsau.4c01206","DOIUrl":"https://doi.org/10.1021/jacsau.4c01206https://doi.org/10.1021/jacsau.4c01206","url":null,"abstract":"<p >Tuberculosis (TB) is an infectious disease caused by <i>Mycobacterium tuberculosis</i> (<i>Mtb</i>), with a complex pathogenesis that poses a long-term threat to human health globally. Early and accurate diagnosis of TB provides a critical window for timely and effective treatment. The development of nucleic acid testing (NAT) based on polymerase chain reaction (PCR) has greatly improved the diagnostic efficiency of TB. However, balancing detection accuracy, efficiency, and cost in TB NAT remains challenging. Functionalized nanomaterials-based nanobiosensors have demonstrated exceptional performance in detecting TB nucleic acid by integrating their unique physicochemical properties with diverse biological probes that exploit Mtb characteristics to effectively amplify biological signals. Compared to traditional NAT, nanobiosensors simplify nucleic acid detection, improve accuracy, and reduce reliance on external conditions, thereby contributing to more immediate and accurate TB diagnosis. In this perspective, we provide a comprehensive summary and discussion on current strategies for detecting <i>Mtb</i> biomarkers using nucleic acid along with novel solutions for TB diagnosis. Additionally, we explore the advantages and challenges associated with applying nanotechnology to the clinical management of TB, particularly point-of-care testing (POCT).</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"536–549 536–549"},"PeriodicalIF":8.5,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c01206","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143473768","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Highly Functional Allyl-Bicyclo[1.1.1]pentane Synthesis by Radical-Initiated Three-Component Stereoselective Allylation","authors":"Qian Zeng,&nbsp;Wangyu Shi and Arjan W. Kleij*,&nbsp;","doi":"10.1021/jacsau.4c0112910.1021/jacsau.4c01129","DOIUrl":"https://doi.org/10.1021/jacsau.4c01129https://doi.org/10.1021/jacsau.4c01129","url":null,"abstract":"<p >Rapid access to highly functional allylated BCP synthons can be achieved with good selectivity and yield through a radical, three-component reaction (3CR) regime using various combinations of radical precursors and vinyl-appended heterocycles acting as versatile and modular precursors. This practical process combines mild operating conditions, a wide scope of reaction partners, and the ability to diversify the functionalized allylic scaffolds further using the allyl and other functional groups as synthetic branching points. The developed protocol allows structural alteration and increases the molecular complexity through late-stage drug modifications and drug conjugation approaches. Mechanistic probes demonstrate that the 3CR process is initiated by a selective, light-promoted radical addition to [1.1.1]-propellane, followed by coupling with the vinyl-substituted heterocycle, which represents a formal decarboxylative radical addition/double bond relay/protonation sequence.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"913–921 913–921"},"PeriodicalIF":8.5,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c01129","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143473866","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Highly Functional Allyl-Bicyclo[1.1.1]pentane Synthesis by Radical-Initiated Three-Component Stereoselective Allylation.","authors":"Qian Zeng, Wangyu Shi, Arjan W Kleij","doi":"10.1021/jacsau.4c01129","DOIUrl":"10.1021/jacsau.4c01129","url":null,"abstract":"<p><p>Rapid access to highly functional allylated BCP synthons can be achieved with good selectivity and yield through a radical, three-component reaction (3CR) regime using various combinations of radical precursors and vinyl-appended heterocycles acting as versatile and modular precursors. This practical process combines mild operating conditions, a wide scope of reaction partners, and the ability to diversify the functionalized allylic scaffolds further using the allyl and other functional groups as synthetic branching points. The developed protocol allows structural alteration and increases the molecular complexity through late-stage drug modifications and drug conjugation approaches. Mechanistic probes demonstrate that the 3CR process is initiated by a selective, light-promoted radical addition to [1.1.1]-propellane, followed by coupling with the vinyl-substituted heterocycle, which represents a formal decarboxylative radical addition/double bond relay/protonation sequence.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"913-921"},"PeriodicalIF":8.5,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11863170/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143525717","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Current Understanding and Translational Prospects of Tetrahedral Framework Nucleic Acids.","authors":"Junjie Gu, Jiale Liang, Taoran Tian, Yunfeng Lin","doi":"10.1021/jacsau.4c01170","DOIUrl":"10.1021/jacsau.4c01170","url":null,"abstract":"<p><p>Tetrahedral framework nucleic acids (tFNAs) represent a promising advancement in nucleic acid nanotechnology due to their unique structural properties, high biocompatibility, and multifaceted biomedical applications. Constructed through a one-pot annealing method, four single-stranded DNAs self-assemble into stable, three-dimensional tetrahedral nanostructures with enhanced mechanical robustness and physiological stability, resisting enzymatic degradation. Their ability to permeate mammalian cells without transfection agents, coupled with modifiable surfaces, positions tFNAs as versatile carriers for drug and gene delivery systems. The tFNA-based platforms exhibit superior therapeutic efficacy, including antioxidative and anti-inflammatory effects, alongside efficient cellular uptake and tissue penetration. These features underpin their role in precision medicine, enabling targeted delivery of diverse therapeutic agents such as synthetic compounds, peptides, and nucleic acids. Additionally, tFNAs demonstrate significant potential in regenerative medicine, immune modulation, antibacterial strategies, and oncology. By addressing challenges in translational integration, tFNAs stand poised to accelerate the development of biomedical research and clinical applications, fostering novel therapies and enhancing therapeutic outcomes across a wide spectrum of diseases. This Perspective thoroughly details the unique attributes and diverse applications of tFNAs and critically evaluates tFNAs' clinical translational potential, outlining inherent implementation challenges and exploring potential solutions to these obstacles.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"486-520"},"PeriodicalIF":8.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11862954/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143525598","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Metabolic PCTA-Based Shift Reagents for the Detection of Extracellular Lactate Using CEST MRI","authors":"Remy Chiaffarelli,&nbsp;Pedro F. Cruz,&nbsp;Jonathan Cotton,&nbsp;Tjark Kelm,&nbsp;Slade Lee,&nbsp;Mohammad Ghaderian,&nbsp;Max Zimmermann,&nbsp;Carlos F. G. C. Geraldes,&nbsp;Paul Jurek and André F. Martins*,&nbsp;","doi":"10.1021/jacsau.4c0102010.1021/jacsau.4c01020","DOIUrl":"https://doi.org/10.1021/jacsau.4c01020https://doi.org/10.1021/jacsau.4c01020","url":null,"abstract":"<p >Lactate is a key metabolic driver in oncology and immunology. Even in the presence of physiological oxygen levels, most cancer cells upregulate anaerobic glycolysis, resulting in abnormal lactate production and accumulation in the tumor microenvironment. The development of more effective, sensitive, and safe probes for detecting extracellular lactate holds the potential to significantly impact cancer metabolic profiling and staging significantly. Macrocyclic-based PARACEST agents have been reported to act as shift reagents (SRs) and detect extracellular lactate via chemical exchange saturation transfer (CEST) MRI. Here, we introduce a new family of SRs based on the PCTA ligand, an inherently stable and kinetically inert group of molecules with the potential for (pre)clinical translation. We observed that Yb-PCTA and Eu-PCTA can significantly shift lactate –OH signals in the CEST spectra. <i>In vitro</i>, CEST MRI experiments proved that imaging extracellular lactate specifically with these complexes is feasible even in the presence of competing small metabolites in blood and in the tumor microenvironment. <i>In vivo</i> preclinical imaging showed that Yb-PCTA can be safely administered intravenously in mice to detect extracellular lactate noninvasively. This work contributes to the field of precision imaging in medicine and provides evidence that the PCTA-ligand is a valuable scaffold for developing molecular and metabolic imaging sensors.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"779–790 779–790"},"PeriodicalIF":8.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c01020","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143473691","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Phenylpyrazoles as Inhibitors of the m6A RNA-Binding Protein YTHDF2","authors":"Xiaqiu Qiu,&nbsp;Claus Kemker,&nbsp;Georg L. Goebel,&nbsp;Philipp Lampe,&nbsp;Nadav Wallis,&nbsp;Damian Schiller,&nbsp;Katrin Bigler,&nbsp;Mao Jiang,&nbsp;Sonja Sievers,&nbsp;Gene W. Yeo and Peng Wu*,&nbsp;","doi":"10.1021/jacsau.4c0075410.1021/jacsau.4c00754","DOIUrl":"https://doi.org/10.1021/jacsau.4c00754https://doi.org/10.1021/jacsau.4c00754","url":null,"abstract":"<p >The <i>N</i>6-methyladenosine (m⁶A) modification, which is the most common RNA modification in eukaryotes, is regulated by the “writer” methyltransferases, the “reader” m⁶A binding proteins, and the “eraser” demethylases. m⁶A plays a multifunctional role in physiological and pathological processes, regulating all aspects of RNA metabolism and function, including RNA splicing, translation, transportation, and degradation. Accumulating evidence suggests that the YT521-B homology domain family 2 (YTHDF2), one of the m⁶A “readers,” is associated with various biological processes in cancers and noncancerous disorders, impacting migration, invasion, metastasis, proliferation, apoptosis, and cell cycle. Here, we describe our work in the identification of a series of functionalized pyrazoles, such as CK-75, as new YTHDF2 inhibitors, which potentially bind to a small hydrophobic pocket on the YTH domain. Cellular evaluations revealed that the small-molecule YTHDF2 inhibitors induced cell cycle arrest, induced apoptosis, and significantly inhibited the cell viability of cancer cells. Furthermore, we evaluated the transcriptome-wide change in the global RNA-binding protein and RNA-binding patterns of CK-75 via an enhanced cross-linking and immunoprecipitation assay. Our work demonstrated the feasibility of targeting the YTH domain of YTHDF2 with small molecules. The phenylpyrazoles studied in this work provided a lead structure for the further development of small molecules targeting YTHDF2 for both biological and therapeutic applications.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"618–630 618–630"},"PeriodicalIF":8.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00754","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143473765","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Prediction of Single-Mutation Effects for Fluorescent Immunosensor Engineering with an End-to-End Trained Protein Language Model.","authors":"Akihito Inoue, Bo Zhu, Keisuke Mizutani, Ken Kobayashi, Takanobu Yasuda, Alon Wellner, Chang C Liu, Tetsuya Kitaguchi","doi":"10.1021/jacsau.4c01189","DOIUrl":"10.1021/jacsau.4c01189","url":null,"abstract":"<p><p>A quenchbody (Q-body) is a fluorophore-labeled homogeneous immunosensor in which the fluorophore is quenched by tryptophan (Trp) residues in the vicinity of the antigen-binding paratope and dequenched in response to antigen binding. Developing Q-bodies against targets on demand remains challenging due to the large sequence space of the complementarity-determining regions (CDRs) related to antigen binding and fluorophore quenching. In this study, we pioneered a strategy using high-throughput screening and a protein language model (pLM) to predict the effects of mutations on fluorophore quenching with single amino acid resolution, thereby enhancing the performance of Q-bodies. We collected yeasts displaying nanobodies with high- and low-quenching properties for the TAMRA fluorophore from a modified large synthetic nanobody library followed by next-generation sequencing. The pretrained pLM, connected to a single-layer perceptron, was trained end-to-end on the enriched CDR sequences. The achieved quenching prediction model that focused on CDR1 + 3 performed best in the evaluation with precision-recall curves. Using this model, we predicted and validated the effective mutations in two anti-SARS-CoV-2 nanobodies, RBD1i13 and RBD10i14, which converted them into Q-bodies. For RBD1i13, three Trp mutants were predicted to have high probability scores for quenching through in silico Trp scanning. These mutants were verified via yeast surface display, and all showed enhanced quenching. For RBD10i14, mutations at four positions close to an existing Trp gave high scores through in silico saturation mutagenesis scanning. Six of eight high-score mutants, derived from two mutants at each of the four positions, exhibited deeper quenching on the yeast surface. Next, combined with the investigation of antigen binding of the mutants, we successfully achieved Q-bodies with enhanced responses. Overall, our strategy allows the prediction of fluorescence responses solely on the basis of the antibody sequence and will be essential for the rational selection and design of antibodies to achieve immunosensors with larger responses.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"955-964"},"PeriodicalIF":8.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11862938/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143525734","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Phenylpyrazoles as Inhibitors of the m⁶A RNA-Binding Protein YTHDF2.","authors":"Xiaqiu Qiu, Claus Kemker, Georg L Goebel, Philipp Lampe, Nadav Wallis, Damian Schiller, Katrin Bigler, Mao Jiang, Sonja Sievers, Gene W Yeo, Peng Wu","doi":"10.1021/jacsau.4c00754","DOIUrl":"10.1021/jacsau.4c00754","url":null,"abstract":"<p><p>The <i>N</i>6-methyladenosine (m⁶A) modification, which is the most common RNA modification in eukaryotes, is regulated by the \"writer\" methyltransferases, the \"reader\" m⁶A binding proteins, and the \"eraser\" demethylases. m⁶A plays a multifunctional role in physiological and pathological processes, regulating all aspects of RNA metabolism and function, including RNA splicing, translation, transportation, and degradation. Accumulating evidence suggests that the YT521-B homology domain family 2 (YTHDF2), one of the m⁶A \"readers,\" is associated with various biological processes in cancers and noncancerous disorders, impacting migration, invasion, metastasis, proliferation, apoptosis, and cell cycle. Here, we describe our work in the identification of a series of functionalized pyrazoles, such as CK-75, as new YTHDF2 inhibitors, which potentially bind to a small hydrophobic pocket on the YTH domain. Cellular evaluations revealed that the small-molecule YTHDF2 inhibitors induced cell cycle arrest, induced apoptosis, and significantly inhibited the cell viability of cancer cells. Furthermore, we evaluated the transcriptome-wide change in the global RNA-binding protein and RNA-binding patterns of CK-75 via an enhanced cross-linking and immunoprecipitation assay. Our work demonstrated the feasibility of targeting the YTH domain of YTHDF2 with small molecules. The phenylpyrazoles studied in this work provided a lead structure for the further development of small molecules targeting YTHDF2 for both biological and therapeutic applications.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"618-630"},"PeriodicalIF":8.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11862924/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143525732","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Current Understanding and Translational Prospects of Tetrahedral Framework Nucleic Acids","authors":"Junjie Gu,&nbsp;Jiale Liang,&nbsp;Taoran Tian* and Yunfeng Lin*,&nbsp;","doi":"10.1021/jacsau.4c0117010.1021/jacsau.4c01170","DOIUrl":"https://doi.org/10.1021/jacsau.4c01170https://doi.org/10.1021/jacsau.4c01170","url":null,"abstract":"<p >Tetrahedral framework nucleic acids (tFNAs) represent a promising advancement in nucleic acid nanotechnology due to their unique structural properties, high biocompatibility, and multifaceted biomedical applications. Constructed through a one-pot annealing method, four single-stranded DNAs self-assemble into stable, three-dimensional tetrahedral nanostructures with enhanced mechanical robustness and physiological stability, resisting enzymatic degradation. Their ability to permeate mammalian cells without transfection agents, coupled with modifiable surfaces, positions tFNAs as versatile carriers for drug and gene delivery systems. The tFNA-based platforms exhibit superior therapeutic efficacy, including antioxidative and anti-inflammatory effects, alongside efficient cellular uptake and tissue penetration. These features underpin their role in precision medicine, enabling targeted delivery of diverse therapeutic agents such as synthetic compounds, peptides, and nucleic acids. Additionally, tFNAs demonstrate significant potential in regenerative medicine, immune modulation, antibacterial strategies, and oncology. By addressing challenges in translational integration, tFNAs stand poised to accelerate the development of biomedical research and clinical applications, fostering novel therapies and enhancing therapeutic outcomes across a wide spectrum of diseases. This Perspective thoroughly details the unique attributes and diverse applications of tFNAs and critically evaluates tFNAs’ clinical translational potential, outlining inherent implementation challenges and exploring potential solutions to these obstacles.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 2","pages":"486–520 486–520"},"PeriodicalIF":8.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c01170","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143473736","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}