In Situ Analytical Techniques for the Investigation of Material Stability and Interface Dynamics in Electrocatalytic and Photoelectrochemical Applications

Pishgar, Sahar; Gulati, Saumya; Strain, Jacob M.; Liang, Ying; Mulvehill, Matthew C.; Spurgeon, Joshua M.

doi:10.1002/smtd.202100322

Cited by 22 publications

(21 citation statements)

References 246 publications

(419 reference statements)

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“…[ 170–172 ] We also suggest analyzing the surface Pourbaix diagrams of SACs before theoretical activity calculations because such analysis can help to determine the most thermodynamically favorable surface states under electrochemical conditions as a function of pH and potential, which leads to much more precise analyses of the mechanism and theoretical activity. [ 173,174 ] For example, our recent surface Pourbaix diagram analysis of NiFe layered double hydroxides found that highly active oxygen vacancies may be formed under alkaline oxygen evolution conditions, as verified by post‐catalytic XPS analysis of the systems. Furthermore, high‐throughput calculations, machine learning, and deep learning could be used to predict potentially catalytically active RE SACs for heterogeneous catalysis by carefully choosing certain key energy descriptors, such as *OH or *O in the ORR and *NH 2 or *HN 2 in the NRR. (4)Extension of practical applications Although RE species display a strong affinity toward oxygen, they could also be used with less electronegative elements, such as S, to weaken the affinity of the RE for adsorbates.…”

Section: Summary and Perspectivesmentioning

confidence: 82%

Rare‐Earth Single‐Atom Catalysts: A New Frontier in Photo/Electrocatalysis

Wang

Zhu

et al. 2022

Small Methods

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through three steps: 1) at the catalyst surface, the reactants diffuse toward the active sites; 2) the reactants are adsorbed at the active sites and transformed into products via consecutive elementary reaction steps; 3) the products diffuse from the surface via chemical desorption. [4][5][6] To facilitate this transformational process, the catalytically active surface should contain many highly catalytically active sites. [7][8][9][10] However, in conventional bulk catalysts, typically, only a few surface atoms provide catalytic activity, and most of the subsurface atoms cannot directly participate in the reactions, thus resulting in atomic waste. [11][12][13][14][15] Recently, more efficient catalysts have been prepared by changing the active sites from those of a bulk catalyst to isolated atoms; these systems are known as single-atom catalysts (SACs). Thus, the term SAC is given to materials whose catalytically active sites are single atoms. The first discussion of SACs can be traced back to 2011, Zhang et al. reported Pt atoms anchored on FeO x (Pt 1 /FeO x ) for CO oxidation. [16] Crucially, when the size of catalysts reaches the atomic scale, distinctive properties that affect their chemical activities, conversion efficiencies, and stabilities emerge. In particular, unlike bulk catalysts, SACs maximize the use of the catalytically active metal atoms (nearly 100% atom efficiency). [17][18][19][20] Further, compared with bulk catalysts, SACs have unique advantages: 1) an unsaturated coordination environment that affects the affinity of the catalyst for intermediate species; 2) distinctive quantum size effects that yield discrete energy levels and frontier molecular orbital (FMO) occupancies; 3) strong atom support interactions that facilitate surface charge redistribution; 4) appropriate polarity to restrain shuttle effects during catalytic processes; 5) breaking of the energy scaling relationship based on the Sabatier principle for enhanced catalytic activity; and 6) site-to-site interactions between single atoms that enhance the catalytic kinetics. [21][22][23][24][25][26][27][28] In recent years, the use of transition-metal-based SACs [29][30][31] and precious-metal-based SACs [32][33][34] has developed rapidly, especially in the field of energy catalysis. In particular, research has focused on Fe, [35][36][37] Co, [38,39] Ni, [40,41] Mn, [42] Pt, [43,44] Ir, [45][46][47] Pd. [48,49] Owing to the strong atom-support interactions, the coupling of the metal and ligand orbitals in the support can result in changes in the d-band center (ε d ) of the metal atoms, [50,51] and this spin-orbit coupling, which results in a range of electronic states, is key to the success of heterogeneous Single-atom catalysts (SACs) provide well-defined active sites with 100% atom utilization, and can be prepared using a wide range of support materials. Therefore, they are attracting global attention, especially in the fields of energy conversion and storage. To date, research has focused on transitionmetal and precious-metal-bas...

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Section: Summary and Perspectivesmentioning

confidence: 82%

Rare‐Earth Single‐Atom Catalysts: A New Frontier in Photo/Electrocatalysis

Wang

Zhu

et al. 2022

Small Methods

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“…The combination of spectroscopic and microscopic imaging can more effectively determine the structural defects in the electrocatalysts. 186,187 For example, tip-enhanced Raman spectroscopy or photoluminescence spectroscopy combined with SEM convey the distribution of defects on the surfaces of the catalysts. 188,189 In addition, the geometric phase analysis (GPA) obtained by the combination of HR-TEM and lattice geometric parameter statistics discloses the geometric distribution of elements, phases, and defects.…”

Section: Microscopic Imaging Methodsmentioning

confidence: 99%

“…The Pt atoms have a higher contrast than the surrounding Co atoms since the atomic number of Pt is larger. The combination of spectroscopic and microscopic imaging can more effectively determine the structural defects in the electrocatalysts 186,187 . For example, tip‐enhanced Raman spectroscopy or photoluminescence spectroscopy combined with SEM convey the distribution of defects on the surfaces of the catalysts 188,189 .…”

Section: Advanced Characterization Of Plasma‐tailored Defective Elect...mentioning

confidence: 99%

“…In electrocatalytic reactions, the microstructure on the catalysts is not static. For example, active sites can fail and migrate and new active sites are constantly generated, 187 as demonstrated in Section 6. Existing in situ characterization techniques have many limitations such as the vacuum environment and insufficient resolution 177,187 .…”

Section: Challenges Opportunities and Future Roadmapmentioning

confidence: 99%

“…For example, active sites can fail and migrate and new active sites are constantly generated, 187 as demonstrated in Section 6. Existing in situ characterization techniques have many limitations such as the vacuum environment and insufficient resolution 177,187 . Therefore, more advanced characterization methods are urgently needed to clarify the principles and paths of various electrocatalytic reactions.…”

Section: Challenges Opportunities and Future Roadmapmentioning

confidence: 99%

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Plasma modified and tailored defective electrocatalysts for water electrolysis and hydrogen fuel cells

Luo

Huang

et al. 2022

EcoMat

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Carbon dioxide generated by the combustion of fossil fuels exacerbates global environmental problems and hydrogen produced by renewable energy is a viable alternative in the continuous transition to sustainable and eco‐conscience development. Electrocatalysts are vital to electrocatalytic reactions and plasma surface modification is one of the promising techniques to modify nanoscale electrocatalysts for water splitting. Up to now, a comprehensive review on the latest developments, challenges, and opportunities of plasma‐tailored defective electrocatalysts for water electrolysis and hydrogen fuel cells is lacking. This paper systematically summarizes the current status of hydrogen production and fuel cell technologies, plasma principles and advantages, plasma‐tailored defective electrocatalysts from the perspective of water splitting and fuel cell applications, advanced characterization of defects, relationship between materials structure and catalytic activity of electrocatalysts, and finally challenges, opportunities, and future roadmap of plasma technologies. This review serves as a reference for future development of hydrogen technologies and offers insights into the structural tailoring of catalytic materials.

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Progress in In Situ Research on Dynamic Surface Reconstruction of Electrocatalysts for Oxygen Evolution Reaction

Shen

Yin

Jin

et al. 2022

Adv Energy and Sustain Res

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Renewable energy and sustainable development have attracted considerable attention due to the rapid growth of energy consumption and environmental pollution. The further development of electrocatalytic water splitting can promote the development and application of next‐generation sustainable energy systems. However, the lack of an in‐depth understanding of the dynamic restructuring process occurring on the catalyst surface in the oxygen evolution reaction (OER) has limited the further development and improvement of OER‐related theories. Therefore, real‐time monitoring and analysis of the dynamic surface reconstruction process has a great significance for deeply understanding the intrinsic catalytic mechanism of OER. Herein, the latest progress on the in situ methods for characterizing the surface reconstruction of various transition metal‐based OER electrocatalysts in recent years is summarized. Many commonly methods used in situ characterization techniques have been reviewed to reveal the correlation between structure, surface reconstruction, and intrinsic activity.

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In Situ Analytical Techniques for the Investigation of Material Stability and Interface Dynamics in Electrocatalytic and Photoelectrochemical Applications

Abstract: Figure 1. Band alignment of photoanode and photocathode semiconductors relative to water oxidation and reduction potentials and material selfoxidation and self-reduction potentials. Reproduced with permission. [12]

Cited by 22 publications

References 246 publications

Rare‐Earth Single‐Atom Catalysts: A New Frontier in Photo/Electrocatalysis

Rare‐Earth Single‐Atom Catalysts: A New Frontier in Photo/Electrocatalysis

Plasma modified and tailored defective electrocatalysts for water electrolysis and hydrogen fuel cells

Progress in In Situ Research on Dynamic Surface Reconstruction of Electrocatalysts for Oxygen Evolution Reaction

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