In situ self-reconstruction inducing amorphous species: A key to electrocatalysis

Liu, Juzhe; Guo, Lin

doi:10.1016/j.matt.2021.05.025

Cited by 70 publications

(45 citation statements)

References 122 publications

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“…Because of the highly oxidative environment, OER catalysts suffer from effects such as spontaneous dissolution and surface reconstruction during operation, which strongly impact the stability of the devices 17 , 18 . These effects in certain cases were also reported to promote the OER activities 19 – 22 . For instance, several research groups reported highly active OER catalysts with perovskite oxide 8 , 23 , nitride 24 , or phoshide 25 as the core materials, and with self-reconstructed amorphous phase or (oxy)hydroxides as the active phase on the surface 18 , 19 , 26 .…”

Section: Introductionmentioning

confidence: 85%

“…These effects in certain cases were also reported to promote the OER activities 19 – 22 . For instance, several research groups reported highly active OER catalysts with perovskite oxide 8 , 23 , nitride 24 , or phoshide 25 as the core materials, and with self-reconstructed amorphous phase or (oxy)hydroxides as the active phase on the surface 18 , 19 , 26 . Jiang et al 27 demonstrated that the leaching of lattice Cl − from cobalt oxychloride (Co 2 (OH) 3 Cl) during the OER process could trigger the atomic-level unsaturated sites and efficiently boost catalytic activity.…”

Section: Introductionmentioning

confidence: 85%

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Activating lattice oxygen in NiFe-based (oxy)hydroxide for water electrolysis

et al. 2022

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Transition metal oxides or (oxy)hydroxides have been intensively investigated as promising electrocatalysts for energy and environmental applications. Oxygen in the lattice was reported recently to actively participate in surface reactions. Herein, we report a sacrificial template-directed approach to synthesize Mo-doped NiFe (oxy)hydroxide with modulated oxygen activity as an enhanced electrocatalyst towards oxygen evolution reaction (OER). The obtained MoNiFe (oxy)hydroxide displays a high mass activity of 1910 A/gmetal at the overpotential of 300 mV. The combination of density functional theory calculations and advanced spectroscopy techniques suggests that the Mo dopant upshifts the O 2p band and weakens the metal-oxygen bond of NiFe (oxy)hydroxide, facilitating oxygen vacancy formation and shifting the reaction pathway for OER. Our results provide critical insights into the role of lattice oxygen in determining the activity of (oxy)hydroxides and demonstrate tuning oxygen activity as a promising approach for constructing highly active electrocatalysts.

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Section: Introductionmentioning

confidence: 85%

Section: Introductionmentioning

confidence: 85%

Activating lattice oxygen in NiFe-based (oxy)hydroxide for water electrolysis

et al. 2022

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“…[33,34] The structural variations undoubtedly have great effect on the electronic properties of these metal oxides and consequently the OER performances. Hence, for OER catalysts, structural variations should be a priority for further mechanism investigation, [35][36][37] and it is essential to establish a complete correlation among the original structural feature, structural variations, the nature of catalytic sites and catalytic performance of metal oxides.…”

Section: Introductionmentioning

confidence: 99%

Structural Variations of Metal Oxide‐Based Electrocatalysts for Oxygen Evolution Reaction

et al. 2021

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including solar, wind, hydro, and biofuel, are highly desired to reduce our reliance on fossil fuels. However, according to the data provided by International Energy Agency, the global energy demand is 120 Mtoe in 2019, most (80%) of which was derived from fossil fuels (coal, natural gas, oil), leading to a huge CO 2 emission (33Gt in 2019). [1][2][3] One of the difficulties hindering the widespread use of these renewable energy sources is their intermittent and unpredictable nature. [4,5] Electrochemical reaction, a promising strategy for converting intermittent electricity into chemical energy, can produce a wide variety of important fuels and chemical feedstock, including hydrogen, hydrocarbons and ammonia. [6][7][8] The feedstocks for these productions obtained from electrochemical reactions can be offered by abundant and universal source, such as water, carbon dioxide and nitrogen. In last decades, due to the net-zero carbon emission features, electrochemical reactions have initiated extensive investigations based on water splitting reaction, nitrogen reduction reaction (NRR) and carbon dioxide reduction reaction. [9][10][11][12] In these green technologies, electrocatalytic oxygen evolution reaction (OER), a core reaction of these process, has a direct impact on device efficiency and cost effectiveness (Figure 1). [13,14] However, OER involves multistep four-electron transferring steps associated with OH breaking and OO formations, thus suffering from sluggish kinetics and requiring a high energy loss (high potential). Therefore, efficient and stable OER electrocatalysts are required to make these renewable energy storage/conversion processes to be viable and scalable technologies. [15,16,221,222] The OER catalysts can be classified into two categories: [17,18] molecular catalysts for homogeneous system and solid catalysts for heterogeneous system. In the homogeneous catalytic system, the molecular catalysts and the electrolyte are in solution, and the OER takes place in the liquid phase. The performance of molecular OER catalysts can be explained and understood at a molecular level by many relatively simple spectroscopic physicochemical techniques. Based on the mechanistic understanding at a molecular level, their geometric and electronic properties are much easier to be fine-tuned to achieve optimum performance by careful selection of the metal ion and ligand environment. Despite all these advantages, molecular catalysts are still not appropriate to be used in practical Electrocatalytic oxygen evolution reaction (OER), an important electrode reaction in electrocatalytic and photoelectrochemical cells for a carbonfree energy cycle, has attracted considerable attention in the last few years. Metal oxides have been considered as good candidates for electrocatalytic OER because they can be easily synthesized and are relatively stable during the OER process. However, inevitable structural variations still occur to them due to the complex reaction steps and harsh working conditions of OER, thus impending the ...

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“…Further prolonging the time of electrolysis, the crystallinity of the shell became worse and the peak intensity became weaker due to that the oxidation reactions caused more and more structural defects and/or disorders on the surface (Figure 4c). [ 29 ] Interestingly, the Co 3 O 4 was very easily formed when the voltage is only 0.2 V from the results of quasi‐operando PXRD under constant voltage electrocatalysis (Figure S31, Supporting Information). It is worth mentioning that the diffraction peaks of cobalt nanoparticles have no significant change with further prolonged electrolysis time or increase of the voltage, indicating that the cobalt nanoparticles in the inner core was not further oxidized after the oxidation reaches an equilibrium, thus forming a stable core‐shell structure (Figure 4d).…”

Section: Resultsmentioning

confidence: 99%

Biodiversity Benefits for Size Modulation of Metal Nanoparticles to Achieve In Situ Semi‐Oxidation toward Optimized Electrocatalytic Oxygen Evolution

Zhang

Sun

Zhang

et al. 2022

Adv Funct Materials

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Biodiversity endows similar species with subtle differences in composition, microstructure, and surface chemistry, making biomass a promising precursor to control the resulting active structure for heterocatalysis. Here, it is shown that Tremella fuciformis (Tfu), possessing an abundant porous structure and favorable metal affinity, is favorably serves as a precursor for confining uniform metal nanoparticles, by comparing the chemical characteristics of six varieties of agarics. The modest size of Co in the Tfu derived composite, Co@NPC‐Tfu (NPC = N, P co‐doped carbon), is suitable for in situ semi‐oxidation during oxygen evolution reaction (OER), forming a stable core‐shell structure of Co3O4@Co. Thus, Co@NPC‐Tfu can be used as a state‐of‐the‐art electrocatalyst for OER with an overpotential of 213.6 ± 4.1 mV at 10 mA cm−2, and a significant turnover frequency of 3.21 s−1 at 300 mV, benefitting from the optimum trade‐off between the atom utilization and electrical conductivity. Operando spectroscopy and theoretical calculations unveil the occupied state modulation of the robust carbon‐bonded POx groups, which optimizes the intermediate adsorption to accelerate OER kinetics. Moreover, Tfu derived Ni@NPC‐Tfu can be also prepared as a high‐performance hydrogen evolution reaction electrocatalyst, which can be utilized for efficient overall water splitting coupled with Co@NPC‐Tfu.

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In situ self-reconstruction inducing amorphous species: A key to electrocatalysis

Cited by 70 publications

References 122 publications

Activating lattice oxygen in NiFe-based (oxy)hydroxide for water electrolysis

Activating lattice oxygen in NiFe-based (oxy)hydroxide for water electrolysis

Structural Variations of Metal Oxide‐Based Electrocatalysts for Oxygen Evolution Reaction

Biodiversity Benefits for Size Modulation of Metal Nanoparticles to Achieve In Situ Semi‐Oxidation toward Optimized Electrocatalytic Oxygen Evolution

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