Steering Single-Site Metallaphotocatalytic Pathway by Accumulated Electron on Carbon Nitride Support DOI

Bangrong Ming,

Tongtong Jia, Yufan Zhang

et al.

Published: Jan. 1, 2023

Organic halide transformation is of high importance for fine chemical synthesis and environmental remediation. Integrated photocatalytic platforms open up distinctive reaction pathway carbon-halogen bond activation/reconstruction. Herein we reveal carbon nitride (CN)-ligated single atom nickel (Ni1/CN), with accumulated electron on the CN, paves Ni-mediated electron-proton transfer, enabling hydrodehalogenation, along catalytic carbon–oxygen (C–O) coupling. The preference hydrodehalogenation positively correlates density CN. EPR measurements suggest photo-generated NiI interacts aryl halides, followed by transfer or reductive elimination to give different products. Further rate law analysis gives distinct orders in substrate (CN) two conversions, unveiling rate-determining step as oxidative addition C–O coupling hydrodehalogenation. Our work advances modulating conversion carrier accumulation photoactive support guides metallaphotocatalytic platform design/operation toward target transformations.

Language: Английский

Advanced carbon nitride‐based single‐atom photocatalysts DOI Creative Commons
Zifan Zhang, Kun Xiang, Haitao Wang

et al.

SusMat, Journal Year: 2024, Volume and Issue: 4(5)

Published: July 18, 2024

Abstract Single‐atom catalysts (SACs) have rapidly become a hot topic in photocatalytic research due to their unique physical and chemical properties, high activity, selectivity. Among many semiconductor carriers, the special structure of carbon nitride (C 3 N 4 ) perfectly meets substrate requirements for stabilizing SACs; they can also compensate defects C materials by modifying energy bands electronic structures. Therefore, developing advanced ‐based SACs is great significance. In this review, we focus on elucidating efficient preparation strategies burgeoning applications SACs. We outline prospective enhancing performance future. A comprehensive array methodologies presented identifying characterizing This includes an exploration potential atomic catalytic mechanisms through simulation regulation behaviors synergistic effects single or multiple sites. Subsequently, forward‐looking perspective adopted contemplate future prospects challenges associated with encompasses considerations, such as loading, regulatory design, integration machine learning techniques. It anticipated that review will stimulate novel insights into synthesis high‐load durable SACs, thereby providing theoretical groundwork scalable controllable field.

Language: Английский

Citations

10
Enrichment of Polarized Alkynes over Negatively Charged Pt for Efficient Electrocatalytic Semihydrogenation DOI
Xiu Lin, Qiyuan Li, Siyuan Xia

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(4), P. 2173 - 2180

Published: Jan. 26, 2024

Semihydrogenation of alkynes is a crucial industrial process for the mass production polymer-grade alkenes and fine chemicals. An electrocatalytic semihydrogenation strategy presents mild but powerful alternative to conventional processes under critical conditions yet suffering from low catalytic efficiency due sacrificed intrinsic activity depress unwanted overhydrogenation. Here, we report negatively charged Pt (Ptδ−) induced by coupling with strong electron donator W2C nanoparticles in dual-junction materials promote using water as hydrogen source. The surface metals enables polarization unexpected preferential enrichment alkynes, accelerating following on real Ptδ−-based electrode. A significantly elevated energy barrier overhydrogenation Ptδ− further ensures selectivity, breaking selectivity-activity trade-off wide scope alkynes. Moreover, Pt-based electrode reusable cathode could exhibit turnover frequency 310 h–1 at −0.4 V versus Ag/AgCl, surpassing 6-fold reported catalysts potential advantages practical applications.

Language: Английский

Citations

9
State-of-the-Art and Perspectives of Nickel-Based Single-Atom Catalysts DOI
Babak Jaleh, Atefeh Nasri, Mahtab Eslamipanah

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124590 - 124590

Published: Sept. 1, 2024

Language: Английский

Citations

7
Insights into the active nickel centers embedded in graphitic carbon nitride for the oxygen evolution reaction DOI Creative Commons
Nicolò Rossetti, Aldo Ugolotti, Claudio Cometto

et al.

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(11), P. 6652 - 6662

Published: Jan. 1, 2024

Combination of experimental work and DFT calculations to establish the structural changes undergone by single Ni atoms stabilized in carbon nitride under OER conditions.

Language: Английский

Citations

4
Efficient Photocatalytic Semihydrogenation of 2-Butyne-1,4-diol over TiO2 Supported Cu Single Atoms with Near-Unity Conversion and Selectivity DOI
Zhenpeng Liu,

Zhipeng Ren,

Jinjin Li

et al.

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

Published: Jan. 8, 2025

Language: Английский

Citations

0
Promotion of Photocatalytic Hydrogen Evolution under Visible Light with NiO/C Fabricated via a Super Facile and General Strategy DOI Creative Commons
Ewa Mijowska, Anna Dymerska, Małgorzata Aleksandrzak

et al.

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(16), P. 6590 - 6599

Published: April 10, 2024

Exploration of efficient, cost-effective, abundant, and environmentally friendly catalysts for generating clean renewable energy resources is currently highly needed. Here, we designed a photocatalyst based on nickel oxide(II) nanoparticles embedded in carbon matrix the photocatalytic hydrogen evolution reaction (pHER). A super facile fabrication strategy involves using only one nontoxic substrate (nickel acetate) as simultaneous source carbon. The catalyst with tuned morphology (via process time) showed superior pHER performance yielding 7.4 mmol/h, an effect synergy between graphitic comes from (i) conductive properties carbon, (ii) defects present matrix, which act sites, (iii) NiO nanoparticles, improve charge carrier separation increasing H2 rate. mechanism was proposed ex situ study postprocessed electron paramagnetic resonance spectroscopy (EPR), X-ray diffraction (XRD), Raman spectroscopy, photoelectron (XPS). What more, propose general simple approach to deliver carbon/metal oxide composites different metal acetates catalytically active materials tunable physicochemical that can meet requirements processes.

Language: Английский

Citations

2
Metal Clusters Effectively Adjust the Local Environment of Polymeric Carbon Nitride for Bifunctional Overall Water Splitting DOI

Anqi Shi,

Wentao Li,

Xiuyun Zhang

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2023, Volume and Issue: 14(44), P. 9804 - 9810

Published: Oct. 27, 2023

Compared with single-atom catalysts, clusters not only possess more metal-loadings and stability but also provide flexible active sites to break the linear scaling relationship of multistep reactions. However, exploring precise structure–activity relationships synergistic effect between nanosheets is still in its infancy. Here, based on first-principles nonequilibrium Green's function simulation, C2N-supported Fe Co tetrahedral exhibit remarkable bifunctional catalytic performance a very low overpotential hydrogen (0.12 0.07 V) /oxygen (0.20 0.55 evolution reactions (HER/OER), respectively. The C2N-regulated have suitable d-band centers around Fermi surface for HER. In turn, activate subadjacent dual-carbon OER. Simultaneously, cluster enhances electronic conductivity C2N, initial current needs ultralow bias voltage 0.1–0.4 V. desired metal regulation strategy offers cost-effective potential advancing clean energy technology.

Language: Английский

Citations

4
Engineered Half-Unit-Cell MoS2/ZnIn2S4 Monolayer Photocatalysts and Adsorbed Hydroxyl Radicals-Assisted Activation of Cα–H Bond for Efficient Cβ–O Bond Cleavage in Lignin to Aromatic Monomers DOI Creative Commons
Zongyang Yue,

Guanchu Lu,

Wenjing Wei

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(36), P. 47724 - 47740

Published: Aug. 31, 2024

Photocatalysis has high potential in the cleavage of C

Language: Английский

Citations

1
Zn-Doped Tubular Graphene Nitride for Visible Light and Sacrificial-Agent-Free H2o2 Photosynthesis in Water DOI

Dexu Zhang,

Xiaoying Peng, Jie Zhang

et al.

Published: Jan. 1, 2024

Language: Английский

Citations

0
Steering Single-Site Metallaphotocatalytic Pathway by Accumulated Electron on Carbon Nitride Support DOI

Bangrong Ming,

Tongtong Jia, Yufan Zhang

et al.

Published: Jan. 1, 2023

Organic halide transformation is of high importance for fine chemical synthesis and environmental remediation. Integrated photocatalytic platforms open up distinctive reaction pathway carbon-halogen bond activation/reconstruction. Herein we reveal carbon nitride (CN)-ligated single atom nickel (Ni1/CN), with accumulated electron on the CN, paves Ni-mediated electron-proton transfer, enabling hydrodehalogenation, along catalytic carbon–oxygen (C–O) coupling. The preference hydrodehalogenation positively correlates density CN. EPR measurements suggest photo-generated NiI interacts aryl halides, followed by transfer or reductive elimination to give different products. Further rate law analysis gives distinct orders in substrate (CN) two conversions, unveiling rate-determining step as oxidative addition C–O coupling hydrodehalogenation. Our work advances modulating conversion carrier accumulation photoactive support guides metallaphotocatalytic platform design/operation toward target transformations.

Language: Английский

Citations

0