Precision ChemistryPub Date : 2025-03-03DOI: 10.1021/prechem.4c0007310.1021/prechem.4c00073
Yudan Chen, Yuanhua Sun, Sicheng Li, Xiaokang Liu, Wei Zhang, Qiquan Luo, Dong Liu*, Tao Ding* and Tao Yao*,
{"title":"Management of Platinum Electronic States through Metal Host–Guest Interactions for Enhanced Oxygen Reduction","authors":"Yudan Chen, Yuanhua Sun, Sicheng Li, Xiaokang Liu, Wei Zhang, Qiquan Luo, Dong Liu*, Tao Ding* and Tao Yao*, ","doi":"10.1021/prechem.4c0007310.1021/prechem.4c00073","DOIUrl":"https://doi.org/10.1021/prechem.4c00073https://doi.org/10.1021/prechem.4c00073","url":null,"abstract":"<p >Controlling the electronic states of Pt-based catalysts holds great promise for enhancing the intrinsic activity of the oxygen reduction reaction (ORR). Herein, inspired by first-principles simulations, we propose a strategy using metal host–guest interactions to tune Pt 5d electronic characteristics to optimize the adsorption strength of the key *OH intermediate. The hybrid electrocatalyst of Pt nanoparticles on a single-atom Co–N–C support (Pt@Co<sub>L</sub> SAs) exhibits a half-wave potential of 0.92 V and a mass activity of 3.2 A·mg<sub>Pt</sub><sup>–1</sup> at 0.9 V in 0.1 M HClO<sub>4</sub>, which is a 20-fold enhancement compared with commercial Pt/C. Impressively, the Pt loading in the catalyst is as low as 1.70 wt %, which represents the lowest value reported in the relevant literature on Pt-based acidic ORR catalysts. Comprehensive spectroscopy investigations and theoretical simulations revealed that the precise regulatory effect of Co in various dispersion states effectively weakens the intermediate adsorption and reduces the energy barrier for the water decomposition step. Our finding provides valuable insights for the development of advanced ultralow-Pt ORR catalysts via the integration engineering of multiple metal sites.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 5","pages":"279–288 279–288"},"PeriodicalIF":0.0,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00073","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133939","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}
Precision ChemistryPub Date : 2025-03-03eCollection Date: 2025-05-26DOI: 10.1021/prechem.4c00073
Yudan Chen, Yuanhua Sun, Sicheng Li, Xiaokang Liu, Wei Zhang, Qiquan Luo, Dong Liu, Tao Ding, Tao Yao
{"title":"Management of Platinum Electronic States through Metal Host-Guest Interactions for Enhanced Oxygen Reduction.","authors":"Yudan Chen, Yuanhua Sun, Sicheng Li, Xiaokang Liu, Wei Zhang, Qiquan Luo, Dong Liu, Tao Ding, Tao Yao","doi":"10.1021/prechem.4c00073","DOIUrl":"10.1021/prechem.4c00073","url":null,"abstract":"<p><p>Controlling the electronic states of Pt-based catalysts holds great promise for enhancing the intrinsic activity of the oxygen reduction reaction (ORR). Herein, inspired by first-principles simulations, we propose a strategy using metal host-guest interactions to tune Pt 5d electronic characteristics to optimize the adsorption strength of the key *OH intermediate. The hybrid electrocatalyst of Pt nanoparticles on a single-atom Co-N-C support (Pt@Co<sub>L</sub> SAs) exhibits a half-wave potential of 0.92 V and a mass activity of 3.2 A·mg<sub>Pt</sub> <sup>-1</sup> at 0.9 V in 0.1 M HClO<sub>4</sub>, which is a 20-fold enhancement compared with commercial Pt/C. Impressively, the Pt loading in the catalyst is as low as 1.70 wt %, which represents the lowest value reported in the relevant literature on Pt-based acidic ORR catalysts. Comprehensive spectroscopy investigations and theoretical simulations revealed that the precise regulatory effect of Co in various dispersion states effectively weakens the intermediate adsorption and reduces the energy barrier for the water decomposition step. Our finding provides valuable insights for the development of advanced ultralow-Pt ORR catalysts via the integration engineering of multiple metal sites.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 5","pages":"279-288"},"PeriodicalIF":0.0,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12117436/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144183422","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}
Tong Ye Wang, Jessica Latimer, Jean-Luc Rukundo, Isaac Kogan, Svetlana M. Krylova, Sebastian Schreiber, Philip Kohlmann, Joachim Jose and Sergey N. Krylov*,
{"title":"","authors":"Tong Ye Wang, Jessica Latimer, Jean-Luc Rukundo, Isaac Kogan, Svetlana M. Krylova, Sebastian Schreiber, Philip Kohlmann, Joachim Jose and Sergey N. Krylov*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 2","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":0.0,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/prechem.4c00085","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144397528","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}
Christopher M. Butch, Patrick C. Hillesheim* and Arsalan Mirjafari*,
{"title":"","authors":"Christopher M. Butch, Patrick C. Hillesheim* and Arsalan Mirjafari*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 2","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":0.0,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/prechem.4c00088","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144397533","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}
Precision ChemistryPub Date : 2025-02-20eCollection Date: 2025-04-28DOI: 10.1021/prechem.4c00102
Cheng Liu, Xu-Yong Chen, Xiao-Jie Cao, Wenmin Zhang, Li-Hui Cao
{"title":"Dual Free Radical Synergism for Enhancing Proton Conductivity in Photochromism iHOFs.","authors":"Cheng Liu, Xu-Yong Chen, Xiao-Jie Cao, Wenmin Zhang, Li-Hui Cao","doi":"10.1021/prechem.4c00102","DOIUrl":"https://doi.org/10.1021/prechem.4c00102","url":null,"abstract":"<p><p>Stimuli-responsive smart materials, as an emerging material, can fulfill reversible transformation of chemical/physical properties under external stimuli such as mechanical stress, light, and electricity, which has the highlights of rapid response, designable structure, and function. Two ionic hydrogen-bonded organic frameworks (<b>iHOFs 36-37</b>) were synthesized by self-assembly of bis(benzene-<i>o</i>/<i>p</i>-sulfonic acid)-naphthalenediimide (<i>o</i>/<i>p</i>-H<sub>2</sub>BSNDI) and two basic ligands. The naphthalenediimide (NDI) was introduced into the material to equip <b>iHOFs 36-37</b> with radical-driven photochromic behavior. The proton conductivity of <b>iHOF-37</b> demonstrated a maximum of 6.50 × 10<sup>-4</sup> S·cm<sup>-1</sup> at 98% RH and 100 °C, and it increased to 9.10 × 10<sup>-3</sup> S·cm<sup>-1</sup> due to dual free radical synergism following UV irradiation (NDI and viologen), which represents a significant 14-fold enhancement. Furthermore, the incorporation of <b>iHOF-37</b> into the chitosan (CS) matrix forms photochromic composite membranes. The proton conductivity of the <b>5%-iHOF-37/CS</b> composite membrane reached up to 5.70 × 10<sup>-2</sup> S·cm<sup>-1</sup> at 98% RH and 90 °C, and reached 8.08 × 10<sup>-2</sup> S·cm<sup>-1</sup> after UV irradiation. This work reveals the dual radicals generated by NDI and viologen derivatives, whose synergistic action plays a significant role in enhancing the proton conductivity in iHOFs and composite membranes, rendering the rational design of stimuli-responsive smart materials feasible.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 4","pages":"221-230"},"PeriodicalIF":0.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12042133/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144050647","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}
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