Construction of graphene oxide-coated zinc tetraphenyporphyrin nanostructures for photocatalytic CO2 reduction to highly selective CH4 product

He, Yiyong; Wang, Zhuoyue; Cao, Aihui; Xu, Xiao; Li, Junqiang; Zhang, Bo; Kang, Longtian

doi:10.1016/j.jcis.2023.01.100

Cited by 14 publications

(2 citation statements)

References 49 publications

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“…The soret (around 420 nm) and Q (500-700 nm) absorption bands in the TPPS electrolyte belong to the π orbitals of the porphyrin ring. [22] It is seen that the soret band underwent a red shift upon chelation of Zn 2 + with TPPS, which could be attributed to the weaker binding affinity of Zn with its outer electrons compared with its coordination with the N atoms in the porphyrin ring. Consequently, the electron cloud density of the π orbital exceeds that of the π* orbital, increasing the electron cloud density of the porphyrin ring and decreasing the energy required for the porphyrin ring's electron transition.…”

Section: Resultsmentioning

confidence: 96%

Tetraphenylporphyrin‐based Chelating Ligand Additive as a Molecular Sieving Interfacial Barrier toward Durable Aqueous Zinc Metal Batteries

Zhao,

Wang,

Huang

et al. 2023

Angew Chem Int Ed

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The sustained water consumption and uncontrollable dendrite growth strongly hamper the practical applications of rechargeable zinc (Zn) metal batteries (ZMBs). Herein, for the first time, we demonstrate that trace amount of chelate ligand additive can serve as a “molecular sieve‐like” interfacial barrier and achieve highly efficient Zn plating/stripping. As verified by theoretical modeling and experimental investigations, the benzenesulfonic acid groups on the additive molecular not only facilitates its water solubility and selective adsorption on the Zn anode, but also effectively accelerates the de‐solvation kinetics of Zn2+. Meanwhile, the central porphyrin ring on the chelate ligand effectively expels free water molecules from Zn2+ via chemical binding against hydrogen evolution, and reversibly releases the captured Zn2+ to endow a dendrite‐free Zn deposition. By virtue of this non‐consumable additive, high average Zn plating/stripping efficiency of 99.7 % over 2100 cycles together with extended lifespan and suppressed water decomposition in the Zn||MnO2 full battery were achieved, thus opening a new avenue for developing highly durable ZMBs.

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Section: Resultsmentioning

confidence: 96%

Tetraphenylporphyrin‐based Chelating Ligand Additive as a Molecular Sieving Interfacial Barrier toward Durable Aqueous Zinc Metal Batteries

Zhao,

Wang,

Huang

et al. 2023

Angew Chem Int Ed

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“…5% def-Nb 2 C/TiO 2 shows the highest CH 4 selectivity of 99.5%, which is much higher than the values reported in the literature and higher than that of TiO 2 . [43][44][45] The accumulation of electrons by the metallic feature of def-Nb 2 C on the surface favors multi-electron reactions. [46,47] However, with 10% def-Nb 2 C, the selectivity to CH 4 decreases, which may be ascribed to the recombination center of def-Nb 2 C at high loading.…”

Section: Introductionmentioning

confidence: 99%

Defective Nb₂C MXene Cocatalyst on TiO₂ Microsphere for Enhanced Photocatalytic CO₂ Conversion to Methane

Yang,

Du,

Deng

et al. 2023

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Sustainable and scalable solar‐energy‐driven CO2 conversion into fuels requires earth‐abundant and stable photocatalysts. In this work, a defective Nb2C MXene as a cocatalyst and TiO2 microspheres as photo‐absorbers, constructed via a coulombic force‐driven self‐assembly, is synthesized. Such photocatalyst, at an optimized loading of defective Nb2C MXene (5% def‐Nb2C/TiO2), exhibits a CH4 production rate of 7.23 µmol g−1 h−1, which is 3.8 times higher than that of TiO2. The Schottky junction at the interface improves charge transfer from TiO2 to defective Nb2C MXene and the electron‐rich feature (nearly free electron states) enables multielectron reaction of CO2, which apparently leads to high activity and selectivity to CH4 (sel. 99.5%) production. Moreover, DFT calculation demonstrates that the Fermi level (EF) of defective Nb2C MXene (−0.3 V vs NHE) is more positive than that of Nb2C MXene (−1.0 V vs NHE), implying a strong capacity to accept photogenerated electrons and enhance carrier lifetime. This work gives a direction to modify the earth‐abundant MXene family as cocatalysts to build high‐performance photocatalysts for energy production.

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Tetraphenylporphyrin‐based Chelating Ligand Additive as a Molecular Sieving Interfacial Barrier toward Durable Aqueous Zinc Metal Batteries

Zhao,

Wang,

Huang

et al. 2023

Angewandte Chemie

View full text Add to dashboard Cite

The sustained water consumption and uncontrollable dendrite growth strongly hamper the practical applications of rechargeable zinc (Zn) metal batteries (ZMBs). Herein, for the first time, we demonstrate that trace amount of chelate ligand additive can serve as a “molecular sieve‐like” interfacial barrier and achieve highly efficient Zn plating/stripping. As verified by theoretical modeling and experimental investigations, the benzenesulfonic acid groups on the additive molecular not only facilitates its water solubility and selective adsorption on the Zn anode, but also effectively accelerates the de‐solvation kinetics of Zn2+. Meanwhile, the central porphyrin ring on the chelate ligand effectively expels free water molecules from Zn2+ via chemical binding against hydrogen evolution, and reversibly releases the captured Zn2+ to endow a dendrite‐free Zn deposition. By virtue of this non‐consumable additive, high average Zn plating/stripping efficiency of 99.7% over 2100 cycles together with extended lifespan and suppressed water decomposition in the Zn||MnO2 full battery were achieved, thus opening a new avenue for developing highly durable ZMBs.

show abstract

Construction of graphene oxide-coated zinc tetraphenyporphyrin nanostructures for photocatalytic CO2 reduction to highly selective CH4 product

Cited by 14 publications

References 49 publications

Tetraphenylporphyrin‐based Chelating Ligand Additive as a Molecular Sieving Interfacial Barrier toward Durable Aqueous Zinc Metal Batteries

Tetraphenylporphyrin‐based Chelating Ligand Additive as a Molecular Sieving Interfacial Barrier toward Durable Aqueous Zinc Metal Batteries

Defective Nb₂C MXene Cocatalyst on TiO₂ Microsphere for Enhanced Photocatalytic CO₂ Conversion to Methane

Tetraphenylporphyrin‐based Chelating Ligand Additive as a Molecular Sieving Interfacial Barrier toward Durable Aqueous Zinc Metal Batteries

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Construction of graphene oxide-coated zinc tetraphenyporphyrin nanostructures for photocatalytic CO2 reduction to highly selective CH4 product

Cited by 14 publications

References 49 publications

Tetraphenylporphyrin‐based Chelating Ligand Additive as a Molecular Sieving Interfacial Barrier toward Durable Aqueous Zinc Metal Batteries

Tetraphenylporphyrin‐based Chelating Ligand Additive as a Molecular Sieving Interfacial Barrier toward Durable Aqueous Zinc Metal Batteries

Defective Nb2C MXene Cocatalyst on TiO2 Microsphere for Enhanced Photocatalytic CO2 Conversion to Methane

Tetraphenylporphyrin‐based Chelating Ligand Additive as a Molecular Sieving Interfacial Barrier toward Durable Aqueous Zinc Metal Batteries

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Defective Nb₂C MXene Cocatalyst on TiO₂ Microsphere for Enhanced Photocatalytic CO₂ Conversion to Methane