High‐Efficiency Oxygen Evolution Reaction: Controllable Reconstruction of Surface Interface DOI Open Access

Lianhui Wu,

Zhixi Guan,

Daying Guo

et al.

Small, Journal Year: 2023, Volume and Issue: 19(49)

Published: Aug. 7, 2023

Abstract The precatalyst undergoes surface reconstruction during the oxygen evolution reaction (OER) process, and reconstituted material is one that really plays a catalytic role. However, degree of seriously affects performance. For this reason, it important to establish link between activity based on deep understanding OER mechanism for rational design high‐performance electrocatalysts. Here, briefly introduced, competition adsorbate (AEM) lattice oxygen‐mediated (LOM) discussed, several descriptors are summarized. strategies realize controllable emphatically including ion leaching, element doping, regulating catalyst size, heterogeneous structure engineering, self‐reconstruction. A mechanistic perspective emphasized understand relationship dynamic electronic structure. Controlled reconfiguration can break limitation proportional brought by traditional AEM mechanism, also switching LOM thus realizing ultra‐low overpotential. This review will provide some reference transition metal‐based catalysts reasonable development ideal

Language: Английский

Unraveling oxygen vacancy site mechanism of Rh-doped RuO2 catalyst for long-lasting acidic water oxidation DOI Creative Commons
Yi Wang, Rong Yang, Yajun Ding

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: March 14, 2023

Exploring durable electrocatalysts with high activity for oxygen evolution reaction (OER) in acidic media is of paramount importance H2 production via polymer electrolyte membrane electrolyzers, yet it remains urgently challenging. Herein, we report a synergistic strategy Rh doping and surface vacancies to precisely regulate unconventional OER path the Ru-O-Rh active sites Rh-RuO2, simultaneously boosting intrinsic stability. The stabilized low-valent catalyst exhibits remarkable performance, an overpotential 161 mV at 10 mA cm-2 retention 99.2% exceeding 700 h 50 cm-2. Quasi situ/operando characterizations demonstrate recurrence reversible species under working potentials enhanced durability. It theoretically revealed that Rh-RuO2 passes through more optimal lattice mediated mechanism-oxygen vacancy site mechanism induced by interaction defects rate-determining step *O formation, breaking barrier limitation (*OOH) traditional adsorption mechanism.

Language: Английский

Citations

241

Reinforcing CoO Covalency via Ce(4f)─O(2p)─Co(3d) Gradient Orbital Coupling for High‐Efficiency Oxygen Evolution DOI
Meng Li,

Xuan Wang,

Kun Liu

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(30)

Published: April 18, 2023

Rare-earth (RE)-based transition metal oxides (TMO) are emerging as a frontier toward the oxygen evolution reaction (OER), yet knowledge regarding their electrocatalytic mechanism and active sites is very limited. In this work, atomically dispersed Ce on CoO successfully designed synthesized by an effective plasma (P)-assisted strategy model (P-Ce SAs@CoO) to investigate origin of OER performance in RE-TMO systems. The P-Ce SAs@CoO exhibits favorable with overpotential only 261 mV at 10 mA cm-2 robust electrochemical stability, superior individual CoO. X-ray absorption spectroscopy situ Raman reveal that Ce-induced electron redistribution inhibits CoO bond breakage CoOCe unit site. Theoretical analysis demonstrates gradient orbital coupling reinforces covalency Ce(4f)─O(2p)─Co(3d) site optimized Co-3d-eg occupancy, which can balance adsorption strength intermediates turn reach apex theoretical maximum, excellent agreement experimental observations. It believed establishment Ce-CoO set basis for mechanistic understanding structural design high-performance catalysts.

Language: Английский

Citations

212

Long‐Term Stability Challenges and Opportunities in Acidic Oxygen Evolution Electrocatalysis DOI
Qilun Wang, Yaqi Cheng, Hua Bing Tao

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(11)

Published: Dec. 22, 2022

Abstract Polymer electrolyte membrane water electrolysis (PEMWE) has been regarded as a promising technology for renewable hydrogen production. However, acidic oxygen evolution reaction (OER) catalysts with long‐term stability impose grand challenge in its large‐scale industrialization. In this review, critical factors that may lead to catalyst's instability couple potential solutions are comprehensively discussed, including mechanical peeling, substrate corrosion, active‐site over‐oxidation/dissolution, reconstruction, oxide crystal structure collapse through the lattice oxygen‐participated pathway, etc. Last but not least, personal prospects provided terms of rigorous evaluation criteria, situ / operando characterizations, economic feasibility and practical electrolyzer consideration, highlighting ternary relationship evolution, industrial‐relevant activity serve roadmap towards ultimate application PEMWE.

Language: Английский

Citations

175

Fundamental Understanding of Structural Reconstruction Behaviors in Oxygen Evolution Reaction Electrocatalysts DOI Creative Commons
Haoyin Zhong, Qi Zhang, Junchen Yu

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(31)

Published: June 29, 2023

Abstract Transition metal‐based oxyhydroxides (MOOH) derived from the irreversible structural reconstruction of precatalysts are often acknowledged as real catalytic species for oxygen evolution reaction (OER). Typically, reconstruction‐derived MOOH would exhibit superior OER activity compared to their directly synthesized counterparts, despite being fundamentally similar in chemistry. As such, has emerged a promising strategy boost electrocatalysts. However, in‐depth understanding origin reconstructed materials still remains ambiguous, which significantly hinders further developments highly efficient electrocatalysts based on In this review, comprehensive overview behaviors reported is provided and intrinsic chemical origins high efficiency toward unveiled. The fundamentals mechanisms, along with recommended characterization techniques dynamic process analyzing structure also interpreted. Finally, view chemistry, potential perspectives facilitate design synthesis durable electrocatalyst presented.

Language: Английский

Citations

157

Coupling Adsorbed Evolution and Lattice Oxygen Mechanism in Fe‐Co(OH)2/Fe2O3 Heterostructure for Enhanced Electrochemical Water Oxidation DOI Creative Commons

Sisi Xin,

Yu Tang, Baohua Jia

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(45)

Published: Sept. 1, 2023

Abstract Oxygen evolution reaction (OER) remains a bottleneck for electrocatalytic water‐splitting to generate hydrogen. However, the traditional adsorbed mechanism (AEM) possesses sluggish kinetics due scaling relationship, while lattice oxygen (LOM) triggers an unstable structure escaping of oxygen. Herein, proof‐of‐concept Fe‐Co(OH) 2 /Fe O 3 heterostructure is put forward, where following AEM can complete rapidly deprotonation process Fe LOM trigger O─O coupling step. Combining theoretical and experimental investigation confirmed that redistributed space‐charge junction optimize synergistically oxygen, facilitate synchronously OER activity stability. As result, shows excellent performance with low overpotential only 219 249 mV reach current density 10 100 mA cm −2 . Specifically, electrocatalyst maintains long‐term stability h at large This work paves avenue break through limit conventional mechanism.

Language: Английский

Citations

120

Optimization of oxygen evolution activity by tuning e*g band broadening in nickel oxyhydroxide DOI
Haoyin Zhong, Xiaopeng Wang, Guangxin Sun

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(2), P. 641 - 652

Published: Jan. 1, 2023

In Ni(OH) 2 , a greater extent of band (3d electron states with e g symmetry) broadening can facilitate transfer from the electrocatalyst to external circuit, leading higher OER catalytic performance.

Language: Английский

Citations

110

Recent Advances on Transition‐Metal‐Based Layered Double Hydroxides Nanosheets for Electrocatalytic Energy Conversion DOI Creative Commons
Yuchen Wang, Man Zhang,

Yaoyu Liu

et al.

Advanced Science, Journal Year: 2023, Volume and Issue: 10(13)

Published: March 3, 2023

Abstract Transition‐metal‐based layered double hydroxides (TM‐LDHs) nanosheets are promising electrocatalysts in the renewable electrochemical energy conversion system, which regarded as alternatives to noble metal‐based materials. In this review, recent advances on effective and facile strategies rationally design TM‐LDHs electrocatalysts, such increasing number of active sties, improving utilization sites (atomic‐scale catalysts), modulating electron configurations, controlling lattice facets, summarized compared. Then, these fabricated for oxygen evolution reaction, hydrogen urea oxidation nitrogen reduction small molecule oxidations, biomass derivatives upgrading is articulated through systematically discussing corresponding fundamental principles reaction mechanism. Finally, existing challenges density catalytically future prospects nanosheets‐based each application also commented.

Language: Английский

Citations

110

Lattice oxygen activation and local electric field enhancement by co-doping Fe and F in CoO nanoneedle arrays for industrial electrocatalytic water oxidation DOI Creative Commons
Pengcheng Ye,

K. Fang,

Haiyan Wang

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 3, 2024

Abstract Oxygen evolution reaction (OER) is critical to renewable energy conversion technologies, but the structure-activity relationships and underlying catalytic mechanisms in catalysts are not fully understood. We herein demonstrate a strategy promote OER with simultaneously achieved lattice oxygen activation enhanced local electric field by dual doping of cations anions. Rough arrays Fe F co-doped CoO nanoneedles constructed, low overpotential 277 mV at 500 mA cm −2 achieved. The dually doped could cooperatively tailor electronic properties CoO, leading improved metal-oxygen covalency stimulated activation. Particularly, induces synergetic effect tip enhancement proximity effect, which effectively concentrates OH − ions, optimizes barrier promotes O 2 desorption. This work demonstrates conceptual couple for effective electrocatalytic water oxidation.

Language: Английский

Citations

110

High‐Entropy Catalyst—A Novel Platform for Electrochemical Water Splitting DOI
Yiyue Zhai, Xiangrong Ren, Bolun Wang

et al.

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(47)

Published: Sept. 16, 2022

Abstract High‐entropy materials (HEMs) have been in the spotlight as emerging catalysts for electrochemical water splitting. In particular, HEM feature multi‐element active sites and unsaturated coordination well entropy stabilization comparison with their single‐element counterparts. Herein, a comprehensive overview of used splitting is provided, covering both hydrogen evolution reaction (HER) oxygen (OER). Particularly, review begins discussions concept structure HEMs. addition, effective strategies rationally designing HEMs on basis computational techniques experimental aspects described. Importantly, importance computationally aided methods, that is, density functional theory calculations, high‐throughput screening, machine learning, to discovery design HEMs, Furthermore, applications field electrolysis are reviewed. Eventually, an outlook regarding prospects future opportunities provided.

Language: Английский

Citations

107

Locking the lattice oxygen in RuO2 to stabilize highly active Ru sites in acidic water oxidation DOI Creative Commons
Xinyu Ping, Yongduo Liu,

Lixia Zheng

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 20, 2024

Abstract Ruthenium dioxide is presently the most active catalyst for oxygen evolution reaction (OER) in acidic media but suffers from severe Ru dissolution resulting high covalency of Ru-O bonds triggering lattice oxidation. Here, we report an interstitial silicon-doping strategy to stabilize highly sites RuO 2 while suppressing The representative Si-RuO −0.1 exhibits activity and stability acid with a negligible degradation rate ~52 μV h −1 800 test overpotential 226 mV at 10 mA cm −2 . Differential electrochemical mass spectrometry (DEMS) results demonstrate that oxidation pathway was suppressed by ∼95% compared commercial , which responsible extraordinary stability. This work supplied unique mentality guide future developments on Ru-based oxide catalysts’ environment.

Language: Английский

Citations

104