Integrating P‐Doped Carbon Nitride Dots as Active Sites on P/Mo Co‐Doped BiVO₄ Photoanodes Promotes H₂O₂ Production

Small, Год журнала: 2025, Номер unknown

Опубликована: Апрель 7, 2025

Abstract The indirect anthraquinone method is currently used to produce H 2 O , but it leads high energy consumption and a large amount of chemical waste. Alternatively, water oxidation reactions offer potential green approach for production, although constrained by low selectivity. Herein, the functional photoanodes are rationally designed production via photocatalytic oxidation. Specifically, P/Mo co‐doped BiVO 4 films achieved on conductive glass serve as layer, which coated with an ultrathin amorphous TiO film achieve good stability. Importantly, metal‐free P‐doped polymeric carbon nitride dots deposited photoanode, acting reaction centres. This innovative moves away from traditional reliance inorganic materials co‐catalysts in order suppress thermodynamically favoured O₂ evolution, which, turn, significantly enhances selectivity, efficiency stability H₂O₂ production. Consequently, optimal selectivity ≈64% at applied voltage bias 1.7 V versus RHE 1.0 m KHCO 3 solution, achieving yield ≈34.2 µmol hr −1 cm −2 . research offers novel strategy developing optimised photoanode synthesis.

Язык: Английский

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Interfacial Hydrogen-Bond Network Regulation Tuned Water Dissociation Enables Selective Chlorination of Alkenes

Journal of the American Chemical Society, Год журнала: 2025, Номер 147(9), С. 8024 - 8031

Опубликована: Фев. 20, 2025

Electrocatalytically selective chlorination of olefins in Cl--containing solutions is a sustainable method for synthesizing chlorohydrin/vicinal dichloride; however, controlling the selectivity challenging. Here, aqueous/dimethyl carbonate (DMC) hybrid electrolytes with different H2O/DMC ratios are designed to modulate ·OH formation increase corresponding selectivities. The combined results in/ex situ spectroscopies and molecular dynamics simulations reveal origin high selectivity. TFSI- shields transportation free H2O provide moderate synthesis chlorohydrin. DMC reconstructs hydrogen bonds minimize interaction between them anode, matching requirements vicinal dichloride production. Thus, these not only achieve selectivities 80% 76% chlorohydrin dichloride, respectively, but also enable other isolated yields up 74%. This work provides facile strategy regulate anodic via rational electrolyte design.

Язык: Английский

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An automatic end-to-end chemical synthesis development platform powered by large language models

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Ноя. 23, 2024

The rapid emergence of large language model (LLM) technology presents promising opportunities to facilitate the development synthetic reactions. In this work, we leveraged power GPT-4 build an LLM-based reaction framework (LLM-RDF) handle fundamental tasks involved throughout chemical synthesis development. LLM-RDF comprises six specialized agents, including Literature Scouter, Experiment Designer, Hardware Executor, Spectrum Analyzer, Separation Instructor, and Result Interpreter, which are pre-prompted accomplish designated tasks. A web application with as backend was built allow chemist users interact automated experimental platforms analyze results via natural language, thus, eliminating need for coding skills ensuring accessibility all chemists. We demonstrated capabilities in guiding end-to-end process copper/TEMPO catalyzed aerobic alcohol oxidation aldehyde reaction, literature search information extraction, substrate scope condition screening, kinetics study, optimization, scale-up product purification. Furthermore, LLM-RDF's broader applicability versability validated on various three distinct reactions (SNAr photoredox C-C cross-coupling heterogeneous photoelectrochemical reaction). rise offers new advancing synthesis. Here, authors developed copilot design

Язык: Английский

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Unexpected piezoelectric properties of electrospun polyimide nanofibers for application in an extreme environment

Journal of Materials Chemistry C, Год журнала: 2024, Номер unknown

Опубликована: Янв. 1, 2024

The piezoelectric properties of FPI nanofibers were first discovered. This makes it a potential material for manufacturing wearable flexible electronic devices in extreme environments.

Язык: Английский

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Upgrading of nitrate to hydrazine through cascading electrocatalytic ammonia production with controllable N-N coupling

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Окт. 3, 2024

Язык: Английский

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Strong adsorption enhances mass transfer and promotes efficient hydrolysis of cellulose to sugar by solid acids

International Journal of Biological Macromolecules, Год журнала: 2024, Номер 279, С. 135060 - 135060

Опубликована: Авг. 28, 2024

Язык: Английский

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Polyfluoroalkanoic Acids as Fluoroalkylating Reagents: Strategy for Direct Access to R_f-Embedded Amides

Organic Letters, Год журнала: 2025, Номер unknown

Опубликована: Янв. 2, 2025

Herein, we have reported the application of bench stable perfluoroalkanoic acids as fluoro-alkylating reagents in combination with DIB and primary amides for sequential one-pot transformation to R

Язык: Английский

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Accelerated flow synthesis of aripiprazole and brexpiprazole in environmentally benign solvents

Green Synthesis and Catalysis, Год журнала: 2025, Номер unknown

Опубликована: Фев. 1, 2025

Язык: Английский

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Electrochemical Conversion of Carboxylic Acids to Terminal Alkenes Enabled by Dialkyl Phosphate Electrolyte

Tetrahedron, Год журнала: 2025, Номер 176, С. 134560 - 134560

Опубликована: Фев. 24, 2025

Язык: Английский

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Photoelectrocatalytic Cl-mediated C(sp3)–H aminomethylation of hydrocarbons by BiVO4 photoanodes

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Март 8, 2025

Interfacial photoelectrochemistry at photoanodes has been extensively researched for solar energy conversion, but its application the production of high-value-added chemical compounds in organic chemistry still presents challenges. Herein, we report photoelectrocatalytic Cl-mediated C(sp3)–H aminomethylation alkanes with self-developed and reusable BiVO4 photoanodes. The swift condensation aniline aldehydes, along decrease electricity input by photogenerated holes photoanodes, work together to prevent excessive oxidation aniline, leading high yields desired product. Mechanistic experiments demonstrate that Cl- ions, as key mediators, could be attracted oxidized form Cl2. This is followed light-promoted homolytic cleavage Cl2, generating Cl radicals efficiently abstract hydrogen atoms from hydrocarbons. opens an avenue interfacial photoelectrochemical synthesis demonstrates a potential method optimizing conversion into fuels. A stable recyclable photoelectrode material was developed efficient hydrocarbons cell, which provides promising fuel conversion.

Язык: Английский

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