Engineering Ultrafast Photo‐Induced Charge and Carbon Intermediates Transfer at Interface to Break the Activity‐Selectivity Trade‐Off in Direct Conversion of Methane to Methanol DOI Open Access
Yuehan Cao, Yu Wang, Yi Li

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 23, 2024

Abstract Directly converting methane to methanol with solar light and eco‐friendly oxidants is challenging due single‐step conversion process where the designed active sites commonly cleave C─H bonds in both methanol. Herein, a novel method proposed break activity‐selectivity trade‐off through interface engineering. Taking BiOI/BN as proof‐of‐concept model, it's discovered that engineered provides distinct for activation overoxidation products photoreduction. Based on situ infrared spectroscopy, ultrafast laser theoretical calculations, it unlocked induces passivation of original trap states BiOI component, greatly hindering trap‐mediated recombination photo‐induced carriers (≈39.7 ps). Benefiting from it, long‐lived electrons could directly participate radicals generation, ensuring effective activation. Subsequently, carbon intermediates protons are captured by BN component rapidly accumulated surface. This enables injection into bonding orbitals methanol, accelerating occurrence re‐bonding process. Ultrafast charge transfer at interfaces results high rate 15.5% under atmospheric pressure maintains selectivity 86.4% 24 h long‐time reaction

Language: Английский

Microwave–Driven Interface Engineering Enhancing Electron Flow for Highly Efficient Solar NO Oxidation over rGO-Integrated NH2-MIL125(Ti)/TiO2 DOI

Xuejian Cheng,

Haotong Ma,

Rong Yang

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: March 1, 2025

Interface design plays a pivotal role in developing high-performance photocatalysts for NO oxidation. In this work, hierarchical rGO-integrated NH2-MIL125(Ti)/TiO2 photocatalyst was constructed using combined liquid-phase and solid-phase microwave synthesis approach. The process enabled the precise deposition of NH2-MIL125(Ti) on graphene oxide (GO), forming strong interfacial bonds, while thermal shock (SMTS) transformed GO into rGO induced formation TiO2 nanoparticles. This structure established an efficient electron transport pathway, promoting charge separation directional transfer to activate O2 generate superoxide radicals (•O2–) as primary reactive species. resulting achieved remarkable oxidation performance, with 81.2% removal efficiency NO3– selectivity 98.5% under simulated sunlight. study highlights potential microwave–driven interface engineering innovative environmentally sustainable applications.

Language: Английский

Citations

1

Highly efficient oxidation of methane into methanol over Ni-promoted Cu/ZSM-5 DOI Creative Commons

Zilong Shen,

Chao Hu,

Jingting Jin

et al.

RSC Advances, Journal Year: 2025, Volume and Issue: 15(11), P. 8244 - 8252

Published: Jan. 1, 2025

Ni-Promoted Cu/ZSM-5 catalyst presented an excellent methanol yield of 82 162 μmol g cat −1 h (with a selectivity ∼74%) in direct conversion methane to methanol.

Language: Английский

Citations

0

Engineering Ultrafast Photo‐Induced Charge and Carbon Intermediates Transfer at Interface to Break the Activity‐Selectivity Trade‐Off in Direct Conversion of Methane to Methanol DOI Open Access
Yuehan Cao, Yu Wang, Yi Li

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 23, 2024

Abstract Directly converting methane to methanol with solar light and eco‐friendly oxidants is challenging due single‐step conversion process where the designed active sites commonly cleave C─H bonds in both methanol. Herein, a novel method proposed break activity‐selectivity trade‐off through interface engineering. Taking BiOI/BN as proof‐of‐concept model, it's discovered that engineered provides distinct for activation overoxidation products photoreduction. Based on situ infrared spectroscopy, ultrafast laser theoretical calculations, it unlocked induces passivation of original trap states BiOI component, greatly hindering trap‐mediated recombination photo‐induced carriers (≈39.7 ps). Benefiting from it, long‐lived electrons could directly participate radicals generation, ensuring effective activation. Subsequently, carbon intermediates protons are captured by BN component rapidly accumulated surface. This enables injection into bonding orbitals methanol, accelerating occurrence re‐bonding process. Ultrafast charge transfer at interfaces results high rate 15.5% under atmospheric pressure maintains selectivity 86.4% 24 h long‐time reaction

Language: Английский

Citations

1