Radical Activation of N–H and O–H Bonds at Bismuth(II)

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(36), С. 16535 - 16544

Опубликована: Сен. 2, 2022

The development of unconventional strategies for the activation ammonia (NH3) and water (H2O) is capital importance advancement sustainable chemical strategies. Herein we provide synthesis characterization a radical equilibrium complex based on bismuth featuring an extremely weak Bi–O bond, which permits in situ generation reactive Bi(II) species. ensuing organobismuth(II) engages with various amines alcohols exerts unprecedented effect onto X–H leading to low BDFEX–H. As result, N–H O–H bonds─including water─occurs seconds at room temperature, delivering well-defined Bi(III)-amido -alkoxy complexes. Moreover, demonstrate that resulting Bi(III)–N complexes engage unique reactivity pattern triad H+, H–, H• sources, thus providing alternative pathways main group chemistry.

Язык: Английский

---

Recent advances in catalytic nitrogen fixation using transition metal–dinitrogen complexes under mild reaction conditions

Coordination Chemistry Reviews, Год журнала: 2022, Номер 472, С. 214783 - 214783

Опубликована: Авг. 26, 2022

Язык: Английский

---

Trends in Electrocatalysis: The Microenvironment Moves to Center Stage

ACS Energy Letters, Год журнала: 2023, Номер 8(9), С. 3935 - 3940

Опубликована: Авг. 28, 2023

ADVERTISEMENT RETURN TO ISSUEPREVEnergy FocusNEXTTrends in Electrocatalysis: The Microenvironment Moves to Center StageMarcel Schreier*Marcel SchreierDepartment of Chemical and Biological Engineering, University Wisconsin-Madison, Madison, Wisconsin 53706, United StatesDepartment Chemistry, States*[email protected]More by Marcel Schreierhttps://orcid.org/0000-0002-3674-5667, Paul KenisPaul KenisDepartment Biomolecular Illinois Urbana-Champaign, Urbana, 61801, StatesMore Kenis, Fanglin CheFanglin CheDepartment Francis College Massachusetts Lowell, One Avenue, 01854, Chehttps://orcid.org/0000-0001-5109-8296, Anthony Shoji Hall*Anthony HallDepartment Materials Science Johns Hopkins University, Baltimore, Maryland 21218, Hallhttps://orcid.org/0000-0003-4134-4160Cite this: ACS Energy Lett. 2023, 8, 9, 3935–3940Publication Date (Web):August 28, 2023Publication History Received6 August 2023Accepted17 2023Published online28 inissue 8 September 2023https://pubs.acs.org/doi/10.1021/acsenergylett.3c01623https://doi.org/10.1021/acsenergylett.3c01623newsACS PublicationsCopyright © Published 2023 American Society. This publication is available under these Terms Use. Request reuse permissions free access through this site. Learn MoreArticle Views5407Altmetric-Citations4LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated reflect usage leading up last few days.Citations number other articles citing article, calculated Crossref daily. Find more information about citation counts.The Altmetric Attention Score a quantitative measure attention that research has received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence for given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InRedditEmail (2 MB) Get e-AlertscloseSUBJECTS:Catalysts,Electrodes,Electrolytes,Ions,Materials e-Alerts

Язык: Английский

---

Mechanical Interlocking Enhances the Electrocatalytic Oxygen Reduction Activity and Selectivity of Molecular Copper Complexes

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(11), С. 6087 - 6099

Опубликована: Фев. 28, 2023

Efficient O2 reduction reaction (ORR) for selective H2O generation enables advanced fuel cell technology. Nonprecious metal catalysts are viable and attractive alternatives to state-of-the-art Pt-based materials that expensive. Cu complexes inspired by Cu-containing enzymes in nature yet reach their desired ORR catalytic performance. Here, the concept of mechanical interlocking is introduced ligand architecture enforce dynamic spatial restriction on coordination site. Interlocked catenane ligands could govern binding mode, promote electron transfer, facilitate product elimination. Our results show as a steers selectivity major via 4e- pathway, rivaling Pt, boosts onset potential 130 mV, mass activity 1.8 times, turnover frequency 1.5 fold compared noninterlocked counterpart. complex represents one first examples take advantage afford electrocatalysts with enhanced selectivity. The mechanistic insights gained through this integrated experimental theoretical study envisioned be valuable not just area energy catalysis but also broad implications interlocked critical importance general fields redox reactions involving proton-coupled transfer steps.

Язык: Английский

---

Redox Mediators in Homogeneous Co-electrocatalysis

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(4), С. 2013 - 2027

Опубликована: Янв. 18, 2023

Homogeneous electrocatalysis has been well studied over the past several decades for conversion of small molecules to useful products green energy applications or as chemical feedstocks. However, in order these catalyst systems be used industrial applications, their activity and stability must improved. In naturally occurring enzymes, redox equivalents (electrons, often a concerted manner with protons) are delivered enzyme active sites by known mediators (RMs). Inspired this, co-electrocatalytic homogeneous catalysts RMs have developed alcohols, nitrogen, unsaturated organic substrates, oxygen, carbon dioxide. systems, shown both increase shift selectivity more desired altering catalytic cycles and/or avoiding high-energy intermediates. area is currently underdeveloped requires additional fundamental advancements become general strategy. Here, we summarize recent examples co-electrocatalysis discuss possible future directions field.

Язык: Английский

---