Stability and deactivation of OER electrocatalysts: A review

Journal of Energy Chemistry, Journal Year: 2022, Volume and Issue: 69, P. 301 - 329

Published: Jan. 29, 2022

Language: Английский

---

Oxygen Evolution/Reduction Reaction Catalysts: From In Situ Monitoring and Reaction Mechanisms to Rational Design

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(9), P. 6257 - 6358

Published: March 21, 2023

The oxygen evolution reaction (OER) and reduction (ORR) are core steps of various energy conversion storage systems. However, their sluggish kinetics, i.e., the demanding multielectron transfer processes, still render OER/ORR catalysts less efficient for practical applications. Moreover, complexity catalyst–electrolyte interface makes a comprehensive understanding intrinsic mechanisms challenging. Fortunately, recent advances in situ/operando characterization techniques have facilitated kinetic monitoring under conditions. Here we provide selected highlights mechanistic studies with main emphasis placed on heterogeneous systems (primarily discussing first-row transition metals which operate basic conditions), followed by brief outlook molecular catalysts. Key sections this review focused determination true active species, identification sites, reactive intermediates. For in-depth insights into above factors, short overview metrics accurate characterizations is provided. A combination obtained time-resolved information reliable activity data will then guide rational design new Strategies such as optimizing restructuring process well overcoming adsorption-energy scaling relations be discussed. Finally, pending current challenges prospects toward development homogeneous presented.

Language: Английский

---

Iron atom–cluster interactions increase activity and improve durability in Fe–N–C fuel cells

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: May 26, 2022

Simultaneously increasing the activity and stability of single-atom active sites M-N-C catalysts is critical but remains a great challenge. Here, we report an Fe-N-C catalyst with nitrogen-coordinated iron clusters closely surrounding Fe-N4 for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction built between satellite due to unblocked electron transfer pathways very short interacting distances. The optimize adsorption strength intermediates on also shorten bond amplitude incoherent vibrations. As result, both are increased by about 60% terms turnover frequency demetalation resistance. This work shows potential interactions multiphase metal species improvements catalysts.

Language: Английский

---

Water splitting performance of metal and non-metal-doped transition metal oxide electrocatalysts

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 474, P. 214864 - 214864

Published: Oct. 12, 2022

Language: Английский

---

Superdurable Bifunctional Oxygen Electrocatalyst for High-Performance Zinc–Air Batteries

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(6), P. 2694 - 2704

Published: Feb. 1, 2022

The development of high-efficiency and durable bifunctional electrocatalysts for both the oxygen reduction reaction (ORR) evolution (OER) is critical widespread application rechargeable zinc-air (Zn-air) batteries. This calls rational screening targeted ORR/OER components precise control their atomic electronic structures to produce synergistic effects. Here, we report a Mn-doped RuO2 (Mn-RuO2) bimetallic oxide with atomic-scale dispersion Mn atoms into lattice, which exhibits remarkable activity super durability ORR OER, very low potential difference (ΔE) 0.64 V between half-wave (E1/2) OER at 10 mA cm-2 (Ej10) negligible decay E1/2 Ej10 after 250 000 30 CV cycles respectively. Moreover, Zn-air batteries using Mn-RuO2 catalysts exhibit high power density 181 mW cm-2, charge/discharge voltage gaps 0.69/0.96/1.38 V, ultralong lifespans 15 000/2800/1800 (corresponding 2500/467/300 h operation time) current 10/50/100 Theoretical calculations reveal that excellent performances mainly due optimization valence state d-band center appropriate adsorption energy oxygenated intermediates.

Language: Английский

---

Progress in Hydrogen Production Coupled with Electrochemical Oxidation of Small Molecules

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(51)

Published: Oct. 6, 2022

Abstract The electrochemical oxidation of small molecules to generate value‐added products has gained enormous interest in recent years because the advantages benign operation conditions, high conversion efficiency and selectivity, absence external oxidizing agents, eco‐friendliness. Coupling replace oxygen evolution reaction (OER) at anode hydrogen (HER) cathode an electrolyzer would simultaneously realize generation high‐value chemicals or pollutant degradation highly efficient production hydrogen. This Minireview presents introduction on small‐molecule choice design strategies electrocatalysts as well breakthroughs achieved Finally, challenges future orientations are highlighted.

Language: Английский

---

Phosphorized CoNi₂S₄ Yolk‐Shell Spheres for Highly Efficient Hydrogen Production via Water and Urea Electrolysis

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(42), P. 22885 - 22891

Published: Aug. 5, 2021

Abstract Exploring earth‐abundant electrocatalysts with excellent activity, robust stability, and multiple functions is crucial for electrolytic hydrogen generation. Porous phosphorized CoNi 2 S 4 yolk‐shell spheres (P‐CoNi YSSs) were rationally designed synthesized by a combined hydrothermal sulfidation gas‐phase phosphorization strategy. Benefiting from the strengthened Ni 3+ /Ni 2+ couple, enhanced electronic conductivity, hollow structure, P‐CoNi YSSs exhibit activity durability towards hydrogen/oxygen evolution urea oxidation reactions in alkaline solution, affording low potentials of −0.135 V, 1.512 1.306 V (versus reversible electrode) at 10 mA cm −2 , respectively. Remarkably, when used as anode cathode simultaneously, catalyst merely requires cell voltage 1.544 water splitting 1.402 electrolysis to attain 100 h, outperforming most reported nickel‐based sulfides even noble‐metal‐based electrocatalysts. This work promotes application electrochemical production provides feasible approach urea‐rich wastewater treatment.

Language: Английский

---

Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

ACS Nano, Journal Year: 2022, Volume and Issue: 16(12), P. 19959 - 19979

Published: Dec. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Language: Английский

---

Metal‐Triazolate‐Framework‐Derived FeN₄Cl₁ Single‐Atom Catalysts with Hierarchical Porosity for the Oxygen Reduction Reaction

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(52), P. 27324 - 27329

Published: Oct. 27, 2021

The construction of single-atom catalysts (SACs) with high single atom densities, favorable electronic structures and fast mass transfer is highly desired. We have utilized metal-triazolate (MET) frameworks, a subclass metal-organic frameworks (MOFs) N content, as precursors since they can enhance the density regulate structure sites, well generate abundant mesopores simultaneously. Fe atoms dispersed in hierarchically porous N-doped carbon matrix metal content (2.78 wt %) FeN4 Cl1 configuration (FeN4 /NC), pore:volume ratio 0.92, were obtained via pyrolysis Zn/Fe-bimetallic MET modified 4,5-dichloroimidazole. /NC exhibits excellent oxygen reduction reaction (ORR) activity both alkaline acidic electrolytes. Density functional theory calculations confirm that Cl optimize adsorption free energy sites to *OH, thereby promoting ORR process. catalyst demonstrates great potential zinc-air batteries. This strategy selects, designs, adjusts MOFs for high-performance SACs.

Language: Английский

---

A durable half-metallic diatomic catalyst for efficient oxygen reduction

Energy & Environmental Science, Journal Year: 2022, Volume and Issue: 15(4), P. 1601 - 1610

Published: Jan. 1, 2022

By elaborately constructing a Fe–Zn based diatomic catalyst, the active center is changed from FeN 4– ZnN 4 to Zn–N 2 after protonation, leading well-maintained structure and thus high stability of ORR.

Language: Английский

---