A living photocatalyst derived from CaCu3Ti4O12 for CO2 hydrogenation to methanol at atmospheric pressure

Jiang, Zaiyong; Yuan, Zhimin; Duchesne, Paul N.; Sun, Wei; Lyu, Xingshuai; Miao, Wenkang; Pérez, Camilo J. Viasus; Xu, Yangfan; Yang, Deren; Huang, Baibiao; Dai, Ying; Wang, Zheng; He, Hong; Ozin, Geoffrey A.

doi:10.1016/j.checat.2023.100507

Cited by 8 publications

(1 citation statement)

References 37 publications

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“…Finally, the population's quality of life is significantly reduced due to damage to Earth's ecosystem. Therefore, finding an environmentally friendly alternative to solve the energy problem is urgently required [8][9][10][11][12]. With its plentiful reservoirs, high specific energy, good combustion characteristics, non-toxicity, non-hazardous, and non-polluting qualities, hydrogen is an extremely effective and clean energy source.…”

Section: Introductionmentioning

confidence: 99%

Sc-Modified C3N4 Nanotubes for High-Capacity Hydrogen Storage: A Theoretical Prediction

Liu,

Tang,

et al. 2024

Molecules

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Utilizing hydrogen as a viable substitute for fossil fuels requires the exploration of hydrogen storage materials with high capacity, high quality, and effective reversibility at room temperature. In this study, the stability and capacity for hydrogen storage in the Sc-modified C3N4 nanotube are thoroughly examined through the application of density functional theory (DFT). Our finding indicates that a strong coupling between the Sc-3d orbitals and N-2p orbitals stabilizes the Sc-modified C3N4 nanotube at a high temperature (500 K), and the high migration barrier (5.10 eV) between adjacent Sc atoms prevents the creation of metal clusters. Particularly, it has been found that each Sc-modified C3N4 nanotube is capable of adsorbing up to nine H2 molecules, and the gravimetric hydrogen storage density is calculated to be 7.29 wt%. It reveals an average adsorption energy of −0.20 eV, with an estimated average desorption temperature of 258 K. This shows that a Sc-modified C3N4 nanotube can store hydrogen at low temperatures and harness it at room temperature, which will reduce energy consumption and protect the system from high desorption temperatures. Moreover, charge donation and reverse transfer from the Sc-3d orbital to the H-1s orbital suggest the presence of the Kubas effect between the Sc-modified C3N4 nanotube and H2 molecules. We draw the conclusion that a Sc-modified C3N4 nanotube exhibits exceptional potential as a stable and efficient hydrogen storage substrate.

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Section: Introductionmentioning

confidence: 99%

Sc-Modified C3N4 Nanotubes for High-Capacity Hydrogen Storage: A Theoretical Prediction

Liu,

Tang,

et al. 2024

Molecules

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Microenvironment Modulation of Ultrathin Bronze‐Phase TiO₂ Nanosheets for Highly Selective Photocatalytic CO₂ Reduction in Water

Jia,

Wan,

Liu

et al. 2023

Adv Funct Materials

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Photocatalytic reduction of CO2 with H2O provides a promising and sustainable pathway to produce valuable chemicals and fuels. However, the low efficiency of CO2 reduction and the concomitant competition of H2 evolution pose serious challenges to practical applications. Herein, a novel approach is proposed to modulate the surface microenvironment of photocatalysts by utilizing hydrogen peroxide (H2O2). A bronze‐phase TiO2 (TB) composed of ultrathin nanosheet with a thickness of ∼3 nm is fabricated and employed as the model catalyst for photocatalytic CO2 reduction. H2O2 molecules are presumed to be bonded to the ultrathin TB surface to form the TB‐H2O2 (TBHO) active specie. The newly generated TBHO enhances the CO2 adsorption and accelerates mass transfer, and the weakly acidic microenvironment of the catalyst surface serves the purpose of mediating the proton‐coupled electron transfer path. Consequently, ultrathin TB nanosheets assisted by H2O2 show an excellent CO generation rate of 29.1 µmol−1 g−1 h−1 (which is 11.2‐fold higher than that of pure TB) in water, and the selectivity toward CO is nearly 100%. This work underscores the importance of tailoring the catalyst surface microenvironment to promote the CO2 reduction while minimizing the H2 generation in pure water.

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Near‐Unity Photothermal CO₂ Hydrogenation to Methanol Based on a Molecule/Nanocarbon Hybrid Catalyst

Ren,

Han,

Yang

et al. 2024

Angewandte Chemie

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Solar‐driven CO2‐to‐methanol conversion provides an intriguing route for both solar energy storage and CO2 mitigation. For scalable applications, near‐unity methanol selectivity is highly desirable to reduce the energy and cost endowed by low‐value byproducts and complex separation processes, but so far has not been achieved. Here we demonstrate a molecule/nanocarbon hybrid catalyst composed of carbon nanotube‐supported molecularly dispersed cobalt phthalocyanine (CoPc/CNT), which synergistically integrates high photothermal conversion capability for affording an optimal reaction temperature with homogeneous and intrinsically‐efficient active sites, to achieve a catalytic activity of 2.4 mmol gcat‐1 h‐1 and selectivity of ~99% in direct photothermal CO2 hydrogenation to methanol reaction. Both theoretical calculations and operando characterizations consistently confirm that the unique electronic structure of CoPc and appropriate reaction temperature cooperatively enable a thermodynamic favorable reaction pathway for highly selective methanol production. This work represents an important milestone towards the development of advanced photothermal catalysts for scalable and cost‐effective CO2 hydrogenation.

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A living photocatalyst derived from CaCu3Ti4O12 for CO2 hydrogenation to methanol at atmospheric pressure

Cited by 8 publications

References 37 publications

Sc-Modified C3N4 Nanotubes for High-Capacity Hydrogen Storage: A Theoretical Prediction

Sc-Modified C3N4 Nanotubes for High-Capacity Hydrogen Storage: A Theoretical Prediction

Microenvironment Modulation of Ultrathin Bronze‐Phase TiO₂ Nanosheets for Highly Selective Photocatalytic CO₂ Reduction in Water

Near‐Unity Photothermal CO₂ Hydrogenation to Methanol Based on a Molecule/Nanocarbon Hybrid Catalyst

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A living photocatalyst derived from CaCu3Ti4O12 for CO2 hydrogenation to methanol at atmospheric pressure

Cited by 8 publications

References 37 publications

Sc-Modified C3N4 Nanotubes for High-Capacity Hydrogen Storage: A Theoretical Prediction

Sc-Modified C3N4 Nanotubes for High-Capacity Hydrogen Storage: A Theoretical Prediction

Microenvironment Modulation of Ultrathin Bronze‐Phase TiO2 Nanosheets for Highly Selective Photocatalytic CO2 Reduction in Water

Near‐Unity Photothermal CO2 Hydrogenation to Methanol Based on a Molecule/Nanocarbon Hybrid Catalyst

Contact Info

Product

Resources

About

Microenvironment Modulation of Ultrathin Bronze‐Phase TiO₂ Nanosheets for Highly Selective Photocatalytic CO₂ Reduction in Water

Near‐Unity Photothermal CO₂ Hydrogenation to Methanol Based on a Molecule/Nanocarbon Hybrid Catalyst