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1.
Proc Natl Acad Sci U S A ; 120(40): e2306673120, 2023 Oct 03.
Artículo en Inglés | MEDLINE | ID: mdl-37748073

RESUMEN

Electrocatalytic nitrogen reduction is a challenging process that requires achieving high ammonia yield rate and reasonable faradaic efficiency. To address this issue, this study developed a catalyst by in situ anchoring interfacial intergrown ultrafine MoO2 nanograins on N-doped carbon fibers. By optimizing the thermal treatment conditions, an abundant number of grain boundaries were generated between MoO2 nanograins, which led to an increased fraction of oxygen vacancies. This, in turn, improved the transfer of electrons, resulting in the creation of highly active reactive sites and efficient nitrogen trapping. The resulting optimal catalyst, MoO2/C700, outperformed commercial MoO2 and state-of-the-art N2 reduction catalysts, with NH3 yield and Faradic efficiency of 173.7 µg h-1 mg-1cat and 27.6%, respectively, under - 0.7 V vs. RHE in 1 M KOH electrolyte. In situ X-ray photoelectron spectroscopy characterization and density functional theory calculation validated the electronic structure effect and advantage of N2 adsorption over oxygen vacancy, revealing the dominant interplay of N2 and oxygen vacancy and generating electronic transfer between nitrogen and Mo(IV). The study also unveiled the origin of improved activity by correlating with the interfacial effect, demonstrating the big potential for practical N2 reduction applications as the obtained optimal catalyst exhibited appreciable catalytic stability during 60 h of continuous electrolysis. This work demonstrates the feasibility of enhancing electrocatalytic nitrogen reduction by engineering grain boundaries to promote oxygen vacancies, offering a promising avenue for efficient and sustainable ammonia production.

2.
Proc Natl Acad Sci U S A ; 120(1): e2209760120, 2023 Jan 03.
Artículo en Inglés | MEDLINE | ID: mdl-36574658

RESUMEN

Using hydrogen as a fuel is an effective way to combat energy crisis and at the same time reduce greenhouse gas emission. Alkaline hydrogen evolution reaction (HER) is one important way to obtain green hydrogen, which however is energy intensive and is difficult to obtain high efficiencies even when using state-of-the-art noble metal catalysts. Here, we report a three-component catalytic system using only non-noble elements, consisting of cobalt oxide clusters and single molybdenum atoms supported on oxyanion-terminated two-dimensional MXene, which enabled the unusual generation of hydrogen by a kinetically fast Volmer-Tafel process in an alkaline electrolyte. The key feature of this catalyst is that the three components are connected by bridging oxygen, which serves to immediately adsorb H* produced during water dissociation on cobalt oxide and relay it to the molybdenum single-atom catalyst. On the Mo atom, due to this unique coordination environment, the relayed H* intermediates directly combine and desorb, realizing H2 generation through an unusual Tafel pathway. The presence of bridging oxygen increases the acidity of the catalyst as Brønsted acid with the reversible adsorption and donation of a proton, thus eliminating the need for acid addition and ensuring excellent and sustainable alkaline HER performance. The performance of our catalyst is comparable to that of the commercial noble metal catalyst PtRu/C. Our work makes a significant contribution to designing efficient non-noble catalysts for alkaline HER electrocatalysis.

3.
Proc Natl Acad Sci U S A ; 119(18): e2202382119, 2022 May 03.
Artículo en Inglés | MEDLINE | ID: mdl-35476529

RESUMEN

SignificanceSeawater is one of the most abundant resources on Earth. Direct electrolysis of seawater is a transformative technology for sustainable hydrogen production without causing freshwater scarcity. However, this technology is severely impeded by a lack of robust and active oxygen evolution reaction (OER) electrocatalysts. Here, we report a highly efficient OER electrocatalyst composed of multimetallic layered double hydroxides, which affords superior catalytic performance and long-term durability for high-performance seawater electrolysis. To the best of our knowledge, this catalyst is among the most active for OER and it advances the development of seawater electrolysis technology.

4.
Nano Lett ; 24(7): 2392-2399, 2024 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-38334492

RESUMEN

Direct electrosynthesis of high-value amino acids from carbon and nitrogen monomers remains a challenge. Here, we design a tandem dual-site PbCu electrocatalyst for efficient amino acid electrosynthesis. Using oxalic acid (H2C2O4) and hydroxylamine (NH2OH) as the raw reactants, for the first time, we have realized the flow-electrosynthesis of glycine at the industrial current density of 200 mA cm-2 with Faradaic efficiency over 78%. In situ ATR-FTIR spectroscopy characterizations reveal a favorable tandem pathway on the dual-site catalyst. Specifically, the Pb site drives the highly selective electroreduction of H2C2O4 to form glyoxylic acid, and the Cu site accelerates the fast hydrogenation of oxime to form a glycine product. A glycine electrosynthesis (GES)-formaldehyde electrooxidation (FOR) assembly is further established, which synthesizes more valuable chemicals (HCOOH, H2) while minimizing energy consumption. Altogether, we introduce a new strategy to enable the one-step electrosynthesis of high-value amino acid from widely accessible monomers.

5.
Nano Lett ; 24(13): 3961-3970, 2024 Apr 03.
Artículo en Inglés | MEDLINE | ID: mdl-38526195

RESUMEN

Developing a high-performance membrane electrode assembly (MEA) poses a formidable challenge for fuel cells, which lies in achieving both high metal loading and efficient catalytic activity concurrently for MEA catalysts. Here, we introduce a porous Co@NC carrier to synthesize sub-4 nm PtCo intermetallic nanocrystals, achieving an impressive Pt loading of 27 wt %. The PtCo-CoNC catalyst demonstrates exceptional catalytic activity and remarkable stability for the oxygen reduction reaction. Advanced characterization techniques and theoretical calculations emphasize the synergistic effect between PtCo alloys and single Co atoms, which enhances the desorption of the OH* intermediate. Furthermore, the PtCo-CoNC-based cathode delivers a high power density of 1.22 W cm-2 in the MEA test owing to the enhanced mass transport, which is verified by the simulation results of the O2 distributions and current density inside the catalyst layer. This study lays the groundwork for the design of efficient catalysts with practical applications in fuel cells.

6.
J Comput Chem ; 45(31): 2602-2611, 2024 Dec 05.
Artículo en Inglés | MEDLINE | ID: mdl-39016463

RESUMEN

Chlorine is an important chemical which has long been produced in chlor-alkali process using dimensionally stable anodes (DSA). However, some serious drawbacks of DSA inspire the development of alternative anodes for chlorine evolution reaction (CER). In this study, we focused on the graphene- and carbon nanotube-supported platinum tetra-phenyl porphyrins as electrocatalysts for CER, which have been theoretically investigated based on density functional theory. Our results reveal that the supported substrates possess potential CER electrocatalytic activity with very low thermodynamic overpotentials (0.012-0.028 V) via Cl* pathway instead of ClO*. The electronic structures analyses showed that electron transfer from the support to the adsorbed chlorine via the Pt center leads to strong Pt-Cl interactions. Furthermore, the supported electrocatalysts exhibited excellent selectivity toward CER because of high overpotentials and reaction barriers of oxygen evolution process. Therefore, our results may pave the way for designing CER electrocatalyst utilizing emerging carbon nanomaterials.

7.
Small ; 20(15): e2308278, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38009756

RESUMEN

Designing cost-efffective electrocatalysts for the oxygen evolution reaction (OER) holds significant importance in the progression of clean energy generation and efficient energy storage technologies, such as water splitting and rechargeable metal-air batteries. In this work, an OER electrocatalyst is developed using Ni and Fe precursors in combination with different proportions of graphene oxide. The catalyst synthesis involved a rapid reduction process, facilitated by adding sodium borohydride, which successfully formed NiFe nanoparticle nests on graphene support (NiFe NNG). The incorporation of graphene support enhances the catalytic activity, electron transferability, and electrical conductivity of the NiFe-based catalyst. The NiFe NNG catalyst exhibits outstanding performance, characterized by a low overpotential of 292.3 mV and a Tafel slope of 48 mV dec-1, achieved at a current density of 10 mA cm- 2. Moreover, the catalyst exhibits remarkable stability over extended durations. The OER performance of NiFe NNG is on par with that of commercial IrO2 in alkaline media. Such superb OER catalytic performance can be attributed to the synergistic effect between the NiFe nanoparticle nests and graphene, which arises from their large surface area and outstanding intrinsic catalytic activity. The excellent electrochemical properties of NiFe NNG hold great promise for further applications in energy storage and conversion devices.

8.
Small ; 20(16): e2309264, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38010948

RESUMEN

In this work, sub-nanometer Co clusters anchored on porous nitrogen-doped carbon (C─N─Co NCs) are successfully prepared by high-temperature annealing and pre-fabricated template strategies for non-invasive sensing of clozapine (CLZ) as an efficient substrate adsorption and electrocatalyst. The introduction of Co sub-nanoclusters (Co NCs) provides enhanced electrochemical performance and better substrate adsorption potential compared to porous and nitrogen-doped carbon structures. Combined with ab initio calculations, it is found that the favorable CLZ catalytic performance with C─N─Co NCs is mainly attributed to possessing a more stable CLZ adsorption structure and lower conversion barriers of CLZ to oxidized state CLZ. An electrochemical sensor for CLZ detection is conceptualized with a wide operating range and high sensitivity, with monitoring capabilities validated in a variety of body fluid environments. Based on the developed CLZ sensing system, the CLZ correlation between blood and saliva and the accuracy of the sensor are investigated by the gold standard method and the rat model of drug administration, paving the way for non-invasive drug monitoring. This work provides new insights into the development of efficient electrocatalysts to enable drug therapy and administration monitoring in personalized healthcare systems.


Asunto(s)
Antipsicóticos , Clozapina , Ratas , Animales , Antipsicóticos/uso terapéutico , Carbono/química , Monitoreo de Drogas , Nitrógeno , Clozapina/química , Clozapina/uso terapéutico
9.
Small ; : e2407495, 2024 Sep 30.
Artículo en Inglés | MEDLINE | ID: mdl-39350444

RESUMEN

The rational design of pH-universal electrocatalyst with high-efficiency, low-cost and large current output suitable for industrial hydrogen evolution reaction (HER) is crucial for hydrogen production via water splitting. Herein, phase engineering of ruthenium (Ru) electrocatalyst comprised of metastable unconventional face-centered cubic (fcc) and conventional hexagonal close-packed (hcp) crystalline phase supported on nitrogen-doped carbon matrix (fcc/hcp-Ru/NC) is successfully synthesized through a facile pyrolysis approach. Fascinatingly, the fcc/hcp-Ru/NC displayed excellent electrocatalytic HER performance under a universal pH range. To deliver a current density of 10 mA cm-2, the fcc/hcp-Ru/NC required overpotentials of 16.8, 23.8 and 22.3 mV in 1 M KOH, 0.5 M H2SO4 and 1 M phosphate buffered solution (PBS), respectively. Even to drive an industrial-level current density of 500 and 1000 mA cm-2, the corresponding overpotentials are 189.8 and 284 mV in alkaline, 202 and 287 mV in acidic media, respectively. Experimental and theoretical calculation result unveiled that the charge migration from fcc-Ru to hcp-Ru induced by work function discrepancy within fcc/hcp-Ru/NC regulate the d-band center of Ru sites, which facilitated the water adsorption and dissociation, thus boosting the electrocatalytic HER performance. The present work paves the way for construction of novel and efficient electrocatalysts for energy conversion and storage.

10.
Small ; : e2406075, 2024 Sep 23.
Artículo en Inglés | MEDLINE | ID: mdl-39314014

RESUMEN

Alkaline electrolysis plays a crucial role in sustainable energy solutions by utilizing electrolytic cells to produce hydrogen gas, providing a clean and efficient method for energy storage and conversion. Efficient, stable, and low-cost electrocatalysts for the oxygen evolution reaction (OER) are essential to facilitate alkaline water electrolysis on a commercial scale. Nickel-iron-based (NiFe-based) transition metal electrocatalysts are considered the most promising non-precious metal catalysts for alkaline OER due to their low cost, abundance, and tunable catalytic properties. Nevertheless, the majority of existing NiFe-based catalysts suffer from limited activity and poor stability, posing a significant challenge in meeting industrial applications. This also highlights a common situation where the emphasis on material activity receives significant attention, while the equally critical stability aspect is often underemphasized. Initiating with a comprehensive exploration of the stability of NiFe-based OER materials, this article first summarizes the debate surrounding the determination of active sites in NiFe-based OER electrocatalysts. Subsequently, the degradation mechanisms of recently reported NiFe-based electrocatalysts are outlined, encompassing assessments of both chemical and mechanical endurance, along with essential approaches for enhancing their stability. Finally, suggestions are put forth regarding the essential considerations for the design of NiFe-based OER electrocatalysts, with a focus on heightened stability.

11.
Small ; : e2406374, 2024 Sep 17.
Artículo en Inglés | MEDLINE | ID: mdl-39285809

RESUMEN

Electrochemiluminescence (ECL) is a powerful tool for clinical diagnosis due to its exceptional sensitivity. However, the standard tripropylamine (TPrA) coreactant for Ru(bpy)3Cl2, the most widely studied and used ECL system, is highly toxic. Despite extensive research on alternative coreactants, they often fall short in poor efficiency. From a reaction kinetics perspective, accelerating electrooxidation rate of Ru(bpy)3Cl2 is an essential way to compensate the efficiency limitation of coreactants, but is rarely reported. Here, a hybrid electrocatalyst@coreactant dots for the ECL of Ru(bpy)3Cl2 is reported. The as-prepared WSe2@bovine serum albumin (WSe2@BSA) dots is biocompatible, and demonstrate dual functions, i.e., the BSA shell works as a coreactant, meanwhile, the WSe2 core effectively catalyzes Ru(bpy)3Cl2 oxidation. As a result, WSe2@BSA dots exhibit an exceptionally high efficiency comparable to TPrA for the ECL of Ru(bpy)3Cl2. In addition, the procedure for synthesizing WSe2@BSA dots is facile (room temperature, atmospheric conditions), rapid (5 min), and scalable (for millions of bioassays). A biosensor utilizing WSe2@BSA dots shows promise for highly sensitive detecting glypican-3 in clinical liver cancer serum samples, especially for alpha-fetoprotein-negative patients. This work opens a new avenue for developing a highly efficient ECL system for biosensing and clinical diagnosis.

12.
Small ; 20(40): e2403170, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-38813750

RESUMEN

Constructing I single-atom (ISA) doped CoP electrocatalyst for HER is extremely challenging and has not been reported to date. Herein, an ISA doping-phosphatization strategy is proposed to prepare a novel I single-atom doped P-rich CoPn nanocluster@CoP electrocatalyst (ISA-CoPn/CoP) with enhanced HER performance first. ISA-CoPn/CoP shows a low overpotential of only 44 and 81 mV in 0.5 m H2SO4 solution, to drive a current density of 10 and 100 mA cm-2. ISA and P-rich CoPn nanocluster show unique synergies, which can optimize the H adsorption energy and accelerate the kinetics of HER in the CoP system. The intermediate I─H bond vibration peak is directly observed through in situ Raman testing, demonstrating that ISA doping helps accelerate the HER process. Additionally, the ΔGH of ISA-CoPn/CoP is only 0.05 eV by density functional theory (DFT) calculation, which is conducive to H2 evolution.

13.
Small ; : e2403415, 2024 Sep 03.
Artículo en Inglés | MEDLINE | ID: mdl-39225396

RESUMEN

Using both density functional theory (DFT+U) simulations and experiments, we show that the incorporation of an ordered array of oxygen-vacancies in a perovskite oxide can lead to enhancement of the electrocatalytic activity for the oxygen-evolution reaction (OER). As a benchmark, LaCoO3 was investigated, where the incorporation of oxygen-vacancies led to La3Co3O8 (LaCoO2.67), featuring a structural transformation. DFT+U simulations demonstrated the effect of oxygen-vacancies on lowering the potential required to achieve negative Gibbs Free Energy for all steps of the OER mechanism. This was also confirmed by experiments, where the vacancy-ordered catalyst La3Co3O8 (LaCoO2.67) showed a remarkable enhancement of electrocatalytic properties over the parent compound LaCoO3 that lacked vacancies. We also synthesized and studied an intermediate system, with a smaller degree of oxygen-vacancies, which showed intermediate electrocatalytic activity, lower than La3Co3O8 and higher than LaCoO3, confirming the expected trend and the impact of oxygen-vacancies. Furthermore, we employed additional DFT+U calculations to simulate a hypothetical material with the same formula as La3Co3O8 but without the vacancy-order. We found that the gap between centers of Co d and O p bands, which is considered an OER descriptor, would be significantly greater for a hypothetical disordered material compared to an ordered system.

14.
Small ; 20(28): e2310786, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38317521

RESUMEN

High-entropy materials have attracted much attention in the electrocatalysis field due to their unique structure, high chemical activity, and compositional tunability. However, the harsh and complex synthetic methods limit the application of such materials. Herein, a universal non-equilibrium liquid-phase synthesis strategy is reported to prepare high-entropy amorphous oxide nanoparticles (HEAO-NPs), and the composition of HEAO-NPs can be precisely controlled from tri- to ten-component. The non-equilibrium synthesis environment provided by an excessively strong reducing agent overcomes the difference in the reduction potentials of various metal ions, resulting in the formation of HEAO-NPs with a nearly equimolar ratio. The oxygen evolution reaction (OER) performance of HEAO-NPs is further improved by adjusting the composition and optimizing the electronic structure. The Fe16Co32Ni32Mn10Cu10BOy exhibits a smaller overpotential (only 259 mV at 10 mA cm-2) and higher stability in OER compared with commercial RuO2. The amorphous high-entropy structure with an optimized concentration of iron makes the binding energy of CoNi shift to a higher direction, promotes the generation of high-valence active intermediates, and accelerates the OER kinetic process. The HEAO-NPs have promising application potential in the field of catalysis, biology, and energy storage, and this work provides a general synthesis method for composition-controllable high-entropy materials.

15.
Small ; : e2404830, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-39148204

RESUMEN

The developed strategies for synthesizing metal phosphides are usually cumbersome and pollute the environment. In this work, an ultrafast (30 s) quasi-solid-state microwave approach is developed to construct cobalt-molybdenum phosphide decorated with Ru (Ru/CoxP-MoP) featured porous morphology with interconnected channels. The specific nanostructure favors mass transport, such as electrolyte bubbles transfer and exposing rich active sites. Moreover, the coupling effects between metallic elements, especially the decorated Ru, also act as a pivotal role on enhancing the electrocatalytic performance. Benefiting from the effects of composition and specific nanostructure, the prepared Ru/CoxP-MoP exhibits efficient HER performance with a current density of 10 mA cm-2 achieved in 1 m KOH, 0.5 m H2SO4, seawater containing 1 m KOH and 1 m PBS, with overpotentials of 52, 59, 55, 90 mV, and coupling with good stability. This work opens a novel and fast avenue to design metal-phosphide-based nanomaterials in energy-conversion and storage fields.

16.
Small ; 20(31): e2401278, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38634520

RESUMEN

Semiconductor-based materials utilized in photocatalysts and electrocatalysts present a sophisticated solution for efficient solar energy utilization and bias control, a field extensively explored for its potential in sustainable energy and environmental management. Recently, 3D printing has emerged as a transformative technology, offering rapid, cost-efficient, and highly customizable approaches to designing photocatalysts and electrocatalysts with precise structural control and tailored substrates. The adaptability and precision of printing facilitate seamless integration, loading, and blending of diverse photo(electro)catalytic materials during the printing process, significantly reducing material loss compared to traditional methods. Despite the evident advantages of 3D printing, a comprehensive compendium delineating its application in the realm of photocatalysis and electrocatalysis is conspicuously absent. This paper initiates by delving into the fundamental principles and mechanisms underpinning photocatalysts electrocatalysts and 3D printing. Subsequently, an exhaustive overview of the latest 3D printing techniques, underscoring their pivotal role in shaping the landscape of photocatalysts and electrocatalysts for energy and environmental applications. Furthermore, the paper examines various methodologies for seamlessly incorporating catalysts into 3D printed substrates, elucidating the consequential effects of catalyst deposition on catalytic properties. Finally, the paper thoroughly discusses the challenges that necessitate focused attention and resolution for future advancements in this domain.

17.
Small ; : e2405784, 2024 Jul 28.
Artículo en Inglés | MEDLINE | ID: mdl-39072920

RESUMEN

The development of efficient, high-performance catalysts for hydrogen evolution reaction (HER) remains a significant challenge, especially in seawater media. Here, RuIr alloy catalysts are prepared by the polyol reduction method. Compared with single-metal catalysts, the RuIr alloy catalysts exhibited higher activity and stability in seawater electrolysis due to their greater number of reactive sites and solubility resistance. The RuIr alloy has an overpotential of 75 mV@10 mA cm-2, which is similar to that of Pt/C (73 mV), and can operate stably for 100 hours in alkaline seawater. Density functional theory (DFT) calculations indicate that hydrogen atoms adsorbed at the top sites of Ru and Ir atoms are more favorable for HER and are most likely to be the reactive sites. This work provides a reference for developing highly efficient and stable catalysts for seawater electrolysis.

18.
Small ; 20(29): e2311929, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38396229

RESUMEN

The global pursuit of sustainable energy is focused on producing hydrogen through electrocatalysis driven by renewable energy. Recently, High entropy alloys (HEAs) have taken the spotlight in electrolysis due to their intriguing cocktail effect, broad design space, customizable electronic structure, and entropy stabilization effect. The tunability and complexity of HEAs allow a diverse range of active sites, optimizing adsorption strength and activity for electrochemical water splitting. This review comprehensively covers contemporary advancements in synthesis technique, design framework, and physio-chemical evaluation approaches for HEA-based electrocatalysts. Additionally, it explores design principles and strategies aimed at optimizing the catalytic activity, stability, and effectiveness of HEAs in hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and overall water splitting. Through an in-depth investigation of these aspects, the complexity inherent in constituent element interactions, reaction processes, and active sites associated with HEAs is aimed to unravel. Eventually, an outlook regarding challenges and impending difficulties and an outline of the future direction of HEA in electrocatalysis is provided. The thorough knowledge offered in this review will assist in formulating and designing catalysts based on HEAs for the next generation of electrochemistry-related applications.

19.
Small ; 20(20): e2309078, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38105404

RESUMEN

Electrocatalytic hydrogen evolution from seawater through wind or solar energy is a cost-effective way to produce green hydrogen fuel. However, the lack of highly active and anti-corrosive electrocatalysts in seawater severely hinders the industrial application. Herein, a novel Ni1.1FeCr0.4V0.3Ti0.3 high-entropy alloy (HEA) is designed through high throughput computing and prepared via powder metallurgy with the surface treated by laser etching under different laser power. The laser-etched NiFeCrVTi high-entropy alloys exhibit a unique periodically ordered structure with multiple active centers and high porosity. The Ni-HEA-30 displays remarkable hydrogen evolution reaction (HER) performance with an overpotential of 55.9 mV and a Tafel slope of 47.3 mV dec-1 in seawater. Density functional theory (DFT) calculations are applied to identify the real active sites for HER on the HEA surface as the key factor for both proton and intermediate transformation, which also reveals that the Cr atom promotes the adsorption energy of water molecules, and the modulation of the electronic structure plays a crucial role in optimizing the hydrogen binding capabilities of the Ni atoms within the alloy. Additionally, the electrocatalyst displays high corrosion resistance in seawater, contributing to the good durability for hydrogen production. This work uncovers a new paradigm to develop novel electrocatalysts with superior reaction activity in seawater.

20.
Small ; : e2403845, 2024 Jun 28.
Artículo en Inglés | MEDLINE | ID: mdl-38940392

RESUMEN

As the anode reaction of proton exchange membrane water electrolysis (PEMWE), the acidic oxygen evolution reaction (OER) is one of the main obstacles to the practical application of PEMWE due to its sluggish four-electron transfer process. The development of high-performance acidic OER electrocatalysts has become the key to improving the reaction kinetics. To date, although various excellent acidic OER electrocatalysts have been widely researched, Ir-based nanomaterials are still state-of-the-art electrocatalysts. Hence, a comprehensive and in-depth understanding of the reaction mechanism of Ir-based electrocatalysts is crucial for the precise optimization of catalytic performance. In this review, the origin and nature of the conventional adsorbate evolution mechanism (AEM) and the derived volcanic relationship on Ir-based electrocatalysts for acidic OER processes are summarized and some optimization strategies for Ir-based electrocatalysts based on the AEM are introduced. To further investigate the development strategy of high-performance Ir-based electrocatalysts, several unconventional OER mechanisms including dual-site mechanism and lattice oxygen mediated mechanism, and their applications are introduced in detail. Thereafter, the active species on Ir-based electrocatalysts at acidic OER are summarized and classified into surface Ir species and O species. Finally, the future development direction and prospect of Ir-based electrocatalysts for acidic OER are put forward.

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