Porous BN with vacancy defects for selective removal of CO from H<sub>2</sub> feed gas in hydrogen fuel cells: a DFT study

Li, Lanlan; Yu, Xiaofei; Yang, Xiaojing; Fang, Yi; Zhang, Xinghua; Xu, Xuewen; Jin, Peng; Tang, Chengchun

doi:10.1039/c6ta03208g

Cited by 30 publications

(8 citation statements)

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“…The strongly interaction indicates that Au atom can be favorably supported on the defect of p-BN in thermodynamics. This is due to so-generated defect states in defective p-BN that affected the system's adsorption ability and catalytic activity (Figure S4) (Li et al, 2016, 2018). In particular, it is found that there is one evident half-occupied d state cross the Fermi level for Au/p-BN-V N (Figure 2B).…”

Section: Resultsmentioning

confidence: 99%

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Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Zhang

et al. 2019

Front. Chem.

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The development of efficient, stable, and low-cost catalytic material for the oxygen reduction reaction (ORR) is currently highly desirable but challenging. In this work, based on first-principles calculation, the stabilities, catalytic activities and catalytic mechanisms of isolated Au atom supported on defective porous BN (p-BN) have been studied in detail. The results reveal that the defective p-BN anchor Au atom strongly to ensure the stability of Au/p-BN. Based on frontier molecular orbital and charge-density analysis, isolated Au atom supported on porous BN with VN defect (Au/p-BN-VN) is an effective ORR catalyst. Especially, the low barriers of the formation (0.38 eV) and dissociation (0.31 eV) of *OOH and the instability of H2O2 on Au/p-BN-VN catalyst suggest that ORR proceeds via 4-electron pathway. Along the favorable pathway, the reduction of O2 to *OOH is the rate-limiting step with the largest activation barrier of 0.38 eV and the maximum free energy change is 1.88 eV. Our results provide a useful guidance for the design and fabrication of new Au-base catalyst with high-efficiency and are beneficial for the developing of novel isolated metal atom catalysts for ORR.

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Section: Resultsmentioning

confidence: 99%

“…As shown in Figure S1, a 3 × 3 × 2 dimension supercell of h-BN was used to construct potential p-BN by introducing vacancies as our previously reported (Li et al, 2016, 2018). The periodic images were separated by a vacuum space of 18 Å in the z direction.…”

Section: Computational Modelsmentioning

confidence: 99%

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Zhang

et al. 2019

Front. Chem.

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“…A 3 × 3 × 2 dimension supercell of h-BN was used to construct potential porous BN by introducing vacancies as previously reported, , with a 15 Å vacuum between sheets to prevent interactions in periodic images. The geometry optimizations were performed using a convergence threshold of 0.001 au/Å on gradients, 0.005 Å on displacements, and 10 –6 au on energy.…”

Section: Models and Methodsmentioning

confidence: 99%

“…Porous boron nitride (p-BN) is a dielectric material similar to porous carbon with a wide band gap of around 4 eV. , The material has unique physical and chemical properties, including high surface area per unit mass, superior total pore volume, elevated ultramicro-porosity, and numerous structural defects. − Importantly, when compared to that of the CC bond, the ionic BN bond may induce an extra dipole moment, which would increase the adsorption energy for gas and ionic molecules. These features render p-BN materials promising candidates for applications in various fields, especially those related to adsorptions of gaseous uptake, pollutants, and catalyst support under very harsh environments. − …”

Section: Introductionmentioning

confidence: 99%

Ambient Carbon Dioxide Capture Using Boron-Rich Porous Boron Nitride: A Theoretical Study

Liu

Yang

et al. 2017

ACS Appl. Mater. Interfaces

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The development of highly efficient sorbent materials for CO capture under ambient conditions is of great importance for reducing the impact of CO on the environment and climate change. In this account, strong CO adsorption on a boron antisite (B) in boron-rich porous boron nitrides (p-BN) was developed and studied. The results indicated that the material achieved larger adsorption energies of 2.09 eV (201.66 kJ/mol, PBE-D). The electronic structure calculations suggested that the introduction of B in p-BN induced defect electronic states in the energy gap region, which strongly impacted the adsorption properties of the material. The bonding between the B defect and the CO molecule was clarified, and it was found that the electron donation first occurred from CO to the B double-acceptor state then, followed by electron back-donation from B to CO accompanied by the formation of a B-C bond. The thermodynamic properties indicated that the adsorption of CO on the B defect to form anionic CO species was spontaneous at temperatures below 350 K. Both the large adsorption energies and the thermodynamic properties ensured that p-BN with a B defect could effectively capture CO under ambient conditions. Finally, to evaluate the energetic stability, the defect formation energies were estimated. The formation energy of the B defects was found to strongly depend on the chemical environment, and the selection of different reactants (B or N sources) would achieve the goal of reducing the formation energy. These findings provided a useful guidance for the design and fabrication of a porous BN sorbent for CO capture.

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“…Graphene can complement the network of electroactive materials to buffer the change in electrode volume and prevent the breakage and aggregation of electrode materials [84][85][86][87]. Density functional theory is the powerful tool electronic structures based on first principles and has been widely used in fuel cells [88]. Mineva et al [89] used density functional theory to study the active sites of Fe-N-C cathode catalysts for fuel cells.…”

Section: Applications Of Graphene-based Nanocomposites In Hydrogen Fu...mentioning

confidence: 99%

Advances in the Applications of Graphene-Based Nanocomposites in Clean Energy Materials

Xiang

Xin

et al. 2021

Crystals

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Extensive use of fossil fuels can lead to energy depletion and serious environmental pollution. Therefore, it is necessary to solve these problems by developing clean energy. Graphene materials own the advantages of high electrocatalytic activity, high conductivity, excellent mechanical strength, strong flexibility, large specific surface area and light weight, thus giving the potential to store electric charge, ions or hydrogen. Graphene-based nanocomposites have become new research hotspots in the field of energy storage and conversion, such as in fuel cells, lithium-ion batteries, solar cells and thermoelectric conversion. Graphene as a catalyst carrier of hydrogen fuel cells has been further modified to obtain higher and more uniform metal dispersion, hence improving the electrocatalyst activity. Moreover, it can complement the network of electroactive materials to buffer the change of electrode volume and prevent the breakage and aggregation of electrode materials, and graphene oxide is also used as a cheap and sustainable proton exchange membrane. In lithium-ion batteries, substituting heteroatoms for carbon atoms in graphene composite electrodes can produce defects on the graphitized surface which have a good reversible specific capacity and increased energy and power densities. In solar cells, the performance of the interface and junction is enhanced by using a few layers of graphene-based composites and more electron-hole pairs are collected; therefore, the conversion efficiency is increased. Graphene has a high Seebeck coefficient, and therefore, it is a potential thermoelectric material. In this paper, we review the latest progress in the synthesis, characterization, evaluation and properties of graphene-based composites and their practical applications in fuel cells, lithium-ion batteries, solar cells and thermoelectric conversion.

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Porous BN with vacancy defects for selective removal of CO from H₂ feed gas in hydrogen fuel cells: a DFT study

Cited by 30 publications

References 40 publications

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Ambient Carbon Dioxide Capture Using Boron-Rich Porous Boron Nitride: A Theoretical Study

Advances in the Applications of Graphene-Based Nanocomposites in Clean Energy Materials

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Porous BN with vacancy defects for selective removal of CO from H2 feed gas in hydrogen fuel cells: a DFT study

Cited by 30 publications

References 40 publications

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Ambient Carbon Dioxide Capture Using Boron-Rich Porous Boron Nitride: A Theoretical Study

Advances in the Applications of Graphene-Based Nanocomposites in Clean Energy Materials

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Porous BN with vacancy defects for selective removal of CO from H₂ feed gas in hydrogen fuel cells: a DFT study