Improved charge separation and surface activation via boron-doped layered polyhedron SrTiO3 for co-catalyst free photocatalytic CO2 conversion

Shan, Jingjing; Raziq, Fazal; Humayun, Muhammad; Zhou, Wei; Qu, Yang; Wang, Guofeng; Li, Yadong

doi:10.1016/j.apcatb.2017.07.024

Cited by 118 publications

(58 citation statements)

References 44 publications

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“…CO 2 -TPD is considered to be sensitive technique to provide detailed information about the interaction between the adsorbed gas molecules and the surface of catalysts. [23] As shown in Figure S21, BIF-29 exhibits one strong desorption peak at 233 8 8Cwhereas BIF-33 displays two weak desorption peaks at about 159 8 8Ca nd 226 8 8C, respectively.T his observation indicates BIF-29 displays relatively stronger CO 2 adsorption active sites compared to BIF-33, although BIF-29 ( Figure S2c) presents smaller amount of adsorbed CO 2 compared to BIF-33 ( Figure S15b), suggesting the catalysis mainly occur at the external surface.Meanwhile, theoretical calculation about CO 2 adsorption energy demonstrated that BIF-29 exhibited more negative adsorption energy of CO 2 compared to BIF-33, suggesting much stronger affinity of BIF-29 with unsaturated coordinated Cu sites towards CO 2 ( Figure S22 and Table S3). [1e,f, 24] Moreover,DFT calculations (Figure 3c)r evealed that for BIF-29, the formation energy of COOH is 1.26 eV for COOH intermediate adsorbed at Cu site.I nc ontrast, for I À -coordinated BIF-33, the COOH intermediate adsorb on Cu site with an extremely high formation energy of 1.63 eV due to the saturated coordination mode of Cu site.T his result indicates that BIF-29 favors the *COOH formation.…”

Section: Angewandte Chemiementioning

confidence: 92%

“…[13] To further reveal the surface-active species,wec arried out in situ electron paramagnetic resonance (EPR) experiments under visible light irradiation. [23] As shown in Figure S21, BIF-29 exhibits one strong desorption peak at 233 8 8Cwhereas BIF-33 displays two weak desorption peaks at about 159 8 8Ca nd 226 8 8C, respectively.T his observation indicates BIF-29 displays relatively stronger CO 2 adsorption active sites compared to BIF-33, although BIF-29 ( Figure S2c) presents smaller amount of adsorbed CO 2 compared to BIF-33 ( Figure S15b), suggesting the catalysis mainly occur at the external surface.Meanwhile, theoretical calculation about CO 2 adsorption energy demonstrated that BIF-29 exhibited more negative adsorption energy of CO 2 compared to BIF-33, suggesting much stronger affinity of BIF-29 with unsaturated coordinated Cu sites towards CO 2 ( Figure S22 and Table S3). Figure S19 indicated that the EPR signal for BIF-29 decrease in density with irradiation time under nitrogen atmosphere.A sacomparison, the EPR signal of Icoordinated BIF-33 keep nearly unchanged.…”

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confidence: 90%

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Isolated Square‐Planar Copper Center in Boron Imidazolate Nanocages for Photocatalytic Reduction of CO₂ to CO

Zhang

Hong

et al. 2019

Angewandte Chemie

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Photocatalytic reduction of CO 2 to value-added fuel has been considered to be apromising strategy to reduce global warming and shortage of energy.Rational design and synthesis of catalysts to maximumly expose the active sites is the key to activate CO 2 molecules and determine the reaction selectivity. Herein, we synthesizeawell-defined copper-based boron imidazolate cage (BIF-29) with six exposed mononuclear copper centers for the photocatalytic reduction of CO 2 . Theoretical calculations show as ingle Cu site including weak coordinated water delivers anew state in the conduction band near the Fermi level and stabilizes the *COOH intermediate. Steady-state and time-resolved fluorescence spectra showthese Cu sites promote the separation of electron-hole pairs and electron transfer.A saresult, the cage achieves solar-driven reduction of CO 2 to CO with an evolution rate of 3334 mmol g À1 h À1 and ahigh selectivity of 82.6 %.With the development of human activities,t he excessive emission of carbon dioxide (CO 2 )r esults in an increasingly serious environmental problem. To address this issue,o ne of the most promising solutions is direct photochemical reduction of CO 2 to useful chemicals or fuels such as methane, methanol, carbon monoxide,and formic acid. [1] Among these possible target products,the two-electron reduction of CO 2 to CO is al ess hindered process and plays an important role in the chemical industry. [1a,2] To date,m uch research has been devoted to developing selective catalysts for reduction of CO 2 to CO. [3] Precious metals have been identified as promising candidates for CO 2 reduction to CO but their practical applications are still limited. Copper as an earth-abundant metal is ac ritical metal in photosynthesis [4] and Cu-based materials have been regarded as promising catalysts for efficiently photo-or electro-catalyzing CO 2 reduction. [5] To date,v arious Cu-based catalysts have been developed but limited product selectivity due to the presence of multiple neighboring sites for involving CO 2 reduction. To enhance product selectivity,aconventional approach is to tailor the number of nearest neighboring accessible Cu atoms,s uch as reducing the particle size [6] or hybridizing Cu with other metals. [7] Besides these,i ntroducing single active site in ac atalyst has been proven to be an effective strategy to study the reactive pathway and enhance the activity for CO 2 reduction reaction (CO2RR). [8] In particular,t he presence of unsaturated coordinated single active sites or defect can modify the electron structure of catalysts,w hich could stabilize the reaction intermediates and thus depress the energy barrier of the photoreduction CO 2 . [9] Recent studies demonstrate that this type of catalyst exhibits high activity for reducing CO 2 to CO. [10] However, such ac atalyst is generally obtained through pyrolysis of Ni, or Co-based metal-organic frameworks (MOFs) or coordination polymers. [10,11] In contrast, no Cu-based catalysts with single active sites have been developed for the pho...

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Section: Angewandte Chemiementioning

confidence: 92%

mentioning

confidence: 90%

Isolated Square‐Planar Copper Center in Boron Imidazolate Nanocages for Photocatalytic Reduction of CO₂ to CO

Zhang

Hong

et al. 2019

Angewandte Chemie

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“…Therefore, the cocatalysts must gather photogenerated charge carriers at specific reaction sites to drive efficient CO 2 photoreduction. Apart from this, Yan et al also reported CO 2 reduction via reversed water gas shift (RWGS) reaction to produce CO, and Shan et al published their work in CO 2 conversion to CH 4

{CO}_{2} + 4 H^{+} + 4 e^{-} \to HCHO + H_{2} normalO E_{o} = - 0.48 normalV vs NHE,

{CO}_{2} + 8 H^{+} + 8 e^{-} \to {CH}_{4} + 2 H_{2} normalO E_{o} = - 0.24 normalV vs NHE .

…”

Section: Applications Of Srtio3mentioning

confidence: 99%

A review of synthesis and morphology of SrTiO ₃ for energy and other applications

et al. 2019

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Summary With the increasing demand and depleting trend of commercial energies, it has forced the researchers all over the world to accelerate research and development in the area of renewable energy. Currently, unique and interesting features of binary compounds have gained more attention by researchers, and it became a favourite research topic among various groups of researchers around this world. It was noticed that strontium titanate (SrTiO3) consists of several extraordinary properties that can apply for miscellaneous applications especially for energy storage, fuel cells, as well as to generate hydrogen fuel via photocatalysis process. Besides that, it was noticed that SrTiO3 can be synthesised in different pathways. The method of preparation and amount of precursors can affect the surface properties of SrTiO3. Thus, this article presents a critical review on how SrTiO3 synthesis methods affect its surface morphology and the applications of SrTiO3 in various fields.

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“…Shan et al [227] used a boron-doped version of SrTiO 3 for photocatalytic conversion of CO 2 . It was reported that the photocatalytic activity of boron-doped SrTiO 3 enhanced by almost 3-fold by the improvement of charge separation potential.…”

Section: Solar Fuelsmentioning

confidence: 99%

Perovskites in the Energy Grid and CO2 Conversion: Current Context and Future Directions

et al. 2020

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CO2 emissions from the consumption of fossil fuels are continuously increasing, thus impacting Earth’s climate. In this context, intensive research efforts are being dedicated to develop materials that can effectively reduce CO2 levels in the atmosphere and convert CO2 into value-added chemicals and fuels, thus contributing to sustainable energy and meeting the increase in energy demand. The development of clean energy by conversion technologies is of high priority to circumvent these challenges. Among the various methods that include photoelectrochemical, high-temperature conversion, electrocatalytic, biocatalytic, and organocatalytic reactions, photocatalytic CO2 reduction has received great attention because of its potential to efficiently reduce the level of CO2 in the atmosphere by converting it into fuels and value-added chemicals. Among the reported CO2 conversion catalysts, perovskite oxides catalyze redox reactions and exhibit high catalytic activity, stability, long charge diffusion lengths, compositional flexibility, and tunable band gap and band edge. This review focuses on recent advances and future prospects in the design and performance of perovskites for CO2 conversion, particularly emphasizing on the structure of the catalysts, defect engineering and interface tuning at the nanoscale, and conversion technologies and rational approaches for enhancing CO2 transformation to value-added chemicals and chemical feedstocks.

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Improved charge separation and surface activation via boron-doped layered polyhedron SrTiO3 for co-catalyst free photocatalytic CO2 conversion

Cited by 118 publications

References 44 publications

Isolated Square‐Planar Copper Center in Boron Imidazolate Nanocages for Photocatalytic Reduction of CO₂ to CO

Isolated Square‐Planar Copper Center in Boron Imidazolate Nanocages for Photocatalytic Reduction of CO₂ to CO

A review of synthesis and morphology of SrTiO ₃ for energy and other applications

Perovskites in the Energy Grid and CO2 Conversion: Current Context and Future Directions

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Improved charge separation and surface activation via boron-doped layered polyhedron SrTiO3 for co-catalyst free photocatalytic CO2 conversion

Cited by 118 publications

References 44 publications

Isolated Square‐Planar Copper Center in Boron Imidazolate Nanocages for Photocatalytic Reduction of CO2 to CO

Isolated Square‐Planar Copper Center in Boron Imidazolate Nanocages for Photocatalytic Reduction of CO2 to CO

A review of synthesis and morphology of SrTiO 3 for energy and other applications

Perovskites in the Energy Grid and CO2 Conversion: Current Context and Future Directions

Contact Info

Product

Resources

About

Isolated Square‐Planar Copper Center in Boron Imidazolate Nanocages for Photocatalytic Reduction of CO₂ to CO

Isolated Square‐Planar Copper Center in Boron Imidazolate Nanocages for Photocatalytic Reduction of CO₂ to CO

A review of synthesis and morphology of SrTiO ₃ for energy and other applications