Pt Atomic Layers with Tensile Strain and Rich Defects Boost Ethanol Electrooxidation

Chen, Yuanjun; Pei, Jiajing; Chen, Zhe; Li, Ang; Ji, Shufang; Rong, Hongpan; Xu, Qian; Wang, Tao; Zhang, Aojie; Tang, Haolin; Zhu, Junfa; Han, Xiao; Zhuang, Zhongbin; Zhou, Gang; Wang, Dingsheng

doi:10.1021/acs.nanolett.2c02572

Cited by 48 publications

(30 citation statements)

References 50 publications

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“…Lattice strain effect is mainly related to the tensile or compressive effect of heterogeneous atoms on bulk atoms, which plays an important role in electrocatalytic reactions by modulating the surface electronic structure of the catalysts and the adsorption capacity of the adsorbate [49][50][51][52][53][54][55] . Recently, by constructing the composition-controllable Pd/Cu core/shell icosahedron, our group proposed a continuous strain regulation strategy to optimize the surface electronic structure and adsorption energy for CO2RR 56 .…”

Section: Lattice Strainmentioning

confidence: 99%

Recent Advances in Defect and Interface Engineering for Electroreduction of CO2 and N2

Chen¹,

Chen²,

Cao³

et al. 2023

Acta Physico Chimica Sinica

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The realization of carbon and nitrogen cycles is an urgent requirement for the development of human society, and is also a hot research topic in the field of catalysis. Electrocatalysis driven by renewable energy has attracted considerable attention, and the target products can be obtained by varying the applied potentials. Accordingly, electrocatalysis is considered to be an effective strategy to alleviate the current energy crisis and environmental problems and is of great significance in realizing carbon neutrality. Electrocatalytic CO2 reduction reaction (CO2RR) and N2 reduction reaction (N2RR) are also promising strategies for the conversion of small molecules. However, the high dissociation energies of the C＝O and N≡N bonds in the linear molecules of CO2 and N2, respectively, lead to their high chemical inactivity. In addition, the large energy gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) further results in high chemical stability. Besides, the low proton affinity of CO2 and N2 makes direct protonated difficult. However, because of the similar redox potentials of CO2RR, N2RR, and hydrogen evolution reaction (HER), HER competes with CO2RR and N2RR, affecting the CO2RR and N2RR performance. Therefore, both CO2RR and N2RR still face challenges, such as high overpotential and low Faradaic efficiency. To overcome these bottlenecks, considerable efforts have been made to improve the performance of the CO2RR and N2RR electrocatalysts. The electrocatalytic process primarily occurs on the catalyst surface and involves mass diffusion and electron transfer; thus, the performance of the catalysts is closely related to their mass and electron transfer abilities. Modulating the catalyst surface structure can regulate the mass and electron transfer behavior of the active sites during the electrocatalytic process. Defect and interface engineering of electrocatalysts is important for enhancing the adsorption of gas, inhibiting HER, enriching the gas, stabilizing the intermediates, and modifying the electronic structure by engineering the surface atoms. To date, various defective and composite electrocatalysts have shown great potential to enhance the CO2RR and N2RR performance. Herein, recent advances in defect and interface engineering for CO2RR and N2RR are reviewed. The effects of four different defects (vacancy, high-index facet, lattice stain, and lattice disorder) on the CO2RR and N2RR performance are discussed. Then, the main roles of interface engineering of polymer-inorganic composite catalysts are further reviewed, and representative examples are presented. Finally, the opportunities and challenges for defect and interface engineering in the electroreduction of CO2 and N2 are also proposed, suggesting directions for the future development of highly efficient CO2RR and N2RR catalysts.

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Section: Lattice Strainmentioning

confidence: 99%

Recent Advances in Defect and Interface Engineering for Electroreduction of CO2 and N2

Chen¹,

Chen²,

Cao³

et al. 2023

Acta Physico Chimica Sinica

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“…Conventional wisdom to address the CO-poisoning issue of Pt electrocatalysts includes alloying Pt with a second metal, − creating composite structures, , engineering surface strain, etc. However, almost no Pt-based catalysts can avoid the formation of CO ad , i.e., they are more or less susceptible to CO poisoning, whether in acidic or alkaline electrolytes.…”

mentioning

confidence: 99%

The Role of Bismuth in Suppressing the CO Poisoning in Alkaline Methanol Electrooxidation: Switching the Reaction from the CO to Formate Pathway

Wang

Liu

et al. 2023

Nano Lett.

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While tuning the electronic structure of Pt can thermodynamically alleviate CO poisoning in direct methanol fuel cells, the impact of interactions between intermediates on the reaction pathway is seldom studied. Herein, we contrive a PtBi model catalyst and realize a complete inhibition of the CO pathway and concurrent enhancement of the formate pathway in the alkaline methanol electrooxidation. The key role of Bi is enriching OH adsorbates (OH ad ) on the catalyst surface. The competitive adsorption of CO adsorbates (CO ad ) and OH ad at Pt sites, complementing the thermodynamic contribution from alloying Bi with Pt, switches the intermediate from CO ad to formate that circumvents CO poisoning. Hence, 8% Bi brings an approximately 6-fold increase in activity compared to pure Pt nanoparticles. This notion can be generalized to modify commercially available Pt/C catalysts by a microwaveassisted method, offering opportunities for the design and practical production of CO-tolerance electrocatalysts in an industrial setting.

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“…That is because the generated defects could regulate the surface electronic structure of Pt and contribute greatly to improving their adsorption capacity for CO intermediate. 62,63 For example, porous PtAg nanoowers have been successfully prepared by combining liquid reduction and chemical etching method. Wang et al rst synthesized different element proportions of PtAg alloys by adjusting the feeding ratios of Pt and Ag precursors, resulting in uneven element distribution.…”

Section: Pt-based Binary Alloysmentioning

confidence: 99%

“…Especially, the surface decoration of Bi(OH) 3 species can accelerate the decomposition of H 2 O to generate OH ad , resulting the removal of CO and other intermediates. 63,121–123 On this basis, porous Pt nanoframes decorated with Bi(OH) 3 species have been prepared by using a two-step method. 124 The porous structure can improve the utilization efficiency of Pt, and Bi(OH) 3 species can enhance the anti-CO poisoning.…”

Section: Pt-based Compositesmentioning

confidence: 99%

Design strategies of Pt-based electrocatalysts and tolerance strategies in fuel cells: a review

Luo¹,

Jiang²,

Wang³

et al. 2023

RSC Adv.

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Pt Atomic Layers with Tensile Strain and Rich Defects Boost Ethanol Electrooxidation

Cited by 48 publications

References 50 publications

Recent Advances in Defect and Interface Engineering for Electroreduction of CO<sub>2</sub> and N<sub>2</sub>

Recent Advances in Defect and Interface Engineering for Electroreduction of CO<sub>2</sub> and N<sub>2</sub>

The Role of Bismuth in Suppressing the CO Poisoning in Alkaline Methanol Electrooxidation: Switching the Reaction from the CO to Formate Pathway

Design strategies of Pt-based electrocatalysts and tolerance strategies in fuel cells: a review

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