Tailoring the Compositions and Nanostructures of Trimetallic Prussian Blue Analog‐Derived Carbides for Water Oxidation DOI Creative Commons

Lujiao Mao,

Jie Liu, Rong Lin

и другие.

Advanced Science, Год журнала: 2024, Номер unknown

Опубликована: Сен. 3, 2024

Abstract The electrochemical splitting of water for hydrogen production faces a major challenge due to its anodic oxygen evolution reaction (OER), necessitating research on the rational design and facile synthesis OER catalysts enhance catalytic activity stability. This study proposes ligand‐induced MOF‐on‐MOF approach fabricate various trimetallic MnFeCo‐based Prussian blue analog (PBA) nanostructures. addition [Fe(CN) 6 ] 3− transforms them from cuboids with protruding corners (MnFeCoPBA‐I) core–shell configurations (MnFeCoPBA‐II), finally hollow structures (MnFeCoPBA‐III). After pyrolysis at 800 °C, they are converted into corresponding PBA‐derived carbon nanomaterials, featuring uniformly dispersed Mn 2 Co C nanoparticles. A comparative analysis demonstrates that Fe enhances activity, while Mn‐doped materials exhibit excellent Specifically, optimized MnFeCoNC‐I‐800 outstanding performance in 1.0 m KOH solution, an overpotential 318 mV 10 mA cm −2 , maintaining stability up 150 h. Theoretical calculations elucidate synergistic interactions between dopants matrix, reducing barriers intermediates improving intrinsic activity. These findings offer valuable insights structure‐morphology relationships MOF precursors, advancing development highly active stable MOF‐derived practical applications.

Язык: Английский

Operando monitoring of the functional role of tetrahedral cobalt centers for the oxygen evolution reaction DOI Creative Commons
Yonggui Zhao, Nanchen Dongfang, Chong Qing Huang

и другие.

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Янв. 10, 2025

The complexity of the intrinsic oxygen evolution reaction (OER) mechanism, particularly precise relationships between local coordination geometry active metal centers and resulting OER kinetics, remains to be fully understood. Herein, we construct a series 3 d transition metal-incorporated cobalt hydroxide-based nanobox architectures for which contain tetrahedrally coordinated Co(II) centers. Combination bulk- surface-sensitive operando spectroelectrochemical approaches reveals that tetrahedral undergo dynamic transformation into highly Co(IV) intermediates acting as true species activate lattice during OER. Such change in Co can further facilitated by partial Fe incorporation. In comparison, formation such is found hindered CoOOH Co-FeOOH, are predominantly containing [CoIIIO6] [CoII/FeIIIO6] octahedra, respectively, but no mono-μ-oxo-bridged [CoIIO4] moieties. This study offers comprehensive view role kinetics. its relationship with center remain unclear. Here, authors report optimization plays crucial facilitating O-O bond atop high-valent (IV) sites.

Язык: Английский

Процитировано

6
The breakthrough of oxide pathway mechanism in stability and scaling relationship for water oxidation DOI Creative Commons
Zhaohua Yin, Hong Liu, Jin‐Song Hu

и другие.

National Science Review, Год журнала: 2024, Номер 11(11)

Опубликована: Окт. 15, 2024

ABSTRACT An in-depth understanding of electrocatalytic mechanisms is essential for advancing electrocatalysts the oxygen evolution reaction (OER). The emerging oxide pathway mechanism (OPM) streamlines direct O–O radical coupling, circumventing formation vacancy defects featured in lattice (LOM) and bypassing additional intermediates (*OOH) inherent to adsorbate (AEM). With only *O *OH as intermediates, OPM-driven stand out their ability disrupt traditional scaling relationships while ensuring stability. This review compiles latest significant advances OPM-based electrocatalysis, detailing design principles, synthetic methods, sophisticated techniques identify active sites pathways. We conclude with prospective challenges opportunities electrocatalysts, aiming advance field into a new era by overcoming constraints.

Язык: Английский

Процитировано

17
Iron‐Induced Localized Oxide Path Mechanism Enables Efficient and Stable Water Oxidation DOI

Bohan Yao,

Yu‐Ting Chen, Yueying Yan

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 6, 2024

Abstract The sluggish reaction kinetics of the anodic oxygen evolution (OER) and inadequate catalytic performance non‐noble metal‐based electrocatalysts represent substantial barriers to development anion exchange membrane water electrolyzer (AEMWE). This study performed synthesis a three‐dimensional (3D) nanoflower‐like electrocatalyst (CFMO) via simple one‐step method. substitution Co with Fe in structure induces localized oxide path mechanism (LOPM), facilitating direct O−O radical coupling for enhanced O 2 evolution. optimized CFMO‐2 demonstrates superior OER performance, achieving an overpotential 217 mV at 10 mA cm −2 , alongside exceptional long‐term stability minimal degradation after 1000 h operation 1.0 M KOH. These properties surpass most conventional noble electrocatalysts. Furthermore, assembled AEMWE system, utilizing CFMO‐2, operates cell voltage 1.65 V deliver A . In situ characterizations reveal that, addition traditional adsorbate (AEM) isolated sites, new LOPM occurred around bimetallic sites. First‐principles calculations confirm greatly reduced energy barriers. work highlights potential improving design AEMWE.

Язык: Английский

Процитировано

15
Two-Dimensional OER Catalysts: Is There a Win-Win Solution for Their Activity and Stability? DOI
Min Ju,

Yu Zhou,

Feng Dong

и другие.

ACS Materials Letters, Год журнала: 2024, Номер unknown, С. 3602 - 3624

Опубликована: Июль 12, 2024

Язык: Английский

Процитировано

13
NiFe‐Based Electrocatalysts for Alkaline Oxygen Evolution: Challenges, Strategies, and Advances Toward Industrial‐Scale Deployment DOI
Yansong Zhou,

Zhitong Wang,

Minghui Cui

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 2, 2024

Abstract Developing high‐efficiency alkaline water splitting technology holds great promise in potentially revolutionizing the traditional petrochemical industry to a more sustainable hydrogen economy. Importantly, oxygen evolution reaction (OER) accompanied at anode is considered as critical bottleneck terms of both complicated mechanism and sluggish kinetics, requiring rational design OER electrocatalysts elucidate structure‐performance relationship reduce applied overpotential. As benchmarked non‐precious metal candidate, NiFe‐based have gained enormous attention due low‐cost, earth‐abundance, remarkable intrinsic activity, which are expected be implemented industrial splitting. In this contribution, comprehensive overview provided, starting with fundamental mechanisms, evaluation metrics, synthetic protocols. Subsequently, basic principles corresponding regulatory strategies summarized following sequence substrate‐catalyst‐electrolyte efficient robust toward industrial‐scale deployment. Perspectives on remaining challenges instructive opportunities booming field finally discussed.

Язык: Английский

Процитировано

13
Engineered Nickel–Iron Nitride Electrocatalyst for Industrial‐Scale Seawater Hydrogen Production DOI
Huashuai Hu,

Xunlu Wang,

Zhaorui Zhang

и другие.

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 25, 2024

Abstract Seawater electrolysis under alkaline conditions is a crucial technology for sustainable hydrogen production. However, achieving the long‐term stability of electrocatalyst remains significant challenge. In this study, it demonstrated that surface reconstruction transition metal nitride (TMN) can be used to develop highly stable oxygen evolution reaction (OER) electrocatalyst. Rapid introduction phosphate groups (PO 4 3− ) accelerates in situ Ni 3 FeN, generating catalyst, with conductive core and Cl − ‐resistant hydroxide shell demonstrates outstanding performance, maintaining over 2500 h at 1 A cm −2 current density seawater. characterization functional theory (DFT) calculations reveal dynamic active sites, providing insights into mechanisms driving stability. This work not only introduces an efficient approach TMN‐based catalyst design but also advances development durable electrocatalysts industrial‐scale seawater

Язык: Английский

Процитировано

11
Regulating Electronic Structure from Local Charge Transfer of Fe-V Dual-sites for Efficient Peroxymonosulfate Activation DOI
Wenlong Wu, Weijie Zhu,

Shouhui Zhao

и другие.

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер unknown, С. 125068 - 125068

Опубликована: Янв. 1, 2025

Язык: Английский

Процитировано

2
Facilitating active NiOOH formation via Mo doping towards high-efficiency oxygen evolution DOI
Liuqing Wang, Jinsheng Li, Qinglei Meng

и другие.

Catalysis Science & Technology, Год журнала: 2024, Номер 14(15), С. 4166 - 4173

Опубликована: Янв. 1, 2024

The promotion effects of Mo doping into NiFe layered double hydroxide were revealed as facilitated NiOOH generation, tailored *OH adsorption, and improved dehydrogenation, which enabled enhanced activity durability towards water oxidation.

Язык: Английский

Процитировано

8
Dual‐Site Bridging Mechanism for Bimetallic Electrochemical Oxygen Evolution DOI
Hongshuai Cao, Xue Wen,

Xianzhu Luo

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(46)

Опубликована: Авг. 9, 2024

Abstract Heterogeneous dual‐site electrocatalysts are emerging cutting‐edge materials for efficient electrochemical water splitting. However, the corresponding oxygen evolution reaction (OER) mechanism on these is still unclear. Herein, based a series of in situ spectroscopy experiments and density function theory (DFT) calculations, new heterogeneous O−O bridging (DSBM) proposed. This to elucidate sequential appearance dual active sites through construction (hybrid ions undergo reconstruction initially), determine crucial role hybrid this (with Ni preferentially adsorbing hydroxyls catalysis followed by proton removal at Fe sites), assess impact bond formation activation state (inducing orderliness activated water), investigate universality Co doping Ni(P 4 O 11 )). Under guidance mechanism, with Fe−Ni(P ) as pre‐catalyst, formed Fe−Ni(OH) 2 electrocatalyst has reached record‐low overpotential 156.4 mV current 18.0 mA cm −2 . Successfully constructed )/Ti uplifting overall efficacy phosphate from moderate superior, positioning it an innovative highly proficient OER.

Язык: Английский

Процитировано

8
Tailoring Non‐Covalent Interaction Via Single Atom to Boost Interfacial Charge Transfer Toward Photoelectrochemical Water Oxidation DOI
Chuanqi Zhang, Yue‐Yue Wang, Wenming Sun

и другие.

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Дек. 4, 2024

Abstract Photoelectrochemical (PEC) water splitting for hydrogen generation holds immense potential addressing environmental and energy crises. Tailoring non‐covalent interaction via a single atom is anticipated to realize prominent hole extracting facilitating PEC performance, but it has never been reported. In this study, Co‐N 4 coordinated with 5‐fluoroanthranilic acid (FAA) molecules, then used as hole‐extracting layer on BiVO substrate. Experiments including X‐ray absorption fine spectra, Kelvin probe force microscopy, transient absorption, theoretical calculation demonstrate the FAA coordination alters local configuration of central Co atom, adjusting interfacial interaction, thereby reducing barrier charge transfer between layer. Consequently, photogenerated carriers are more effectively separated, oxidation performance significantly enhanced photocurrent density 5.47 mA cm −2 at 1.23 V versus RHE, much higher than those previously reported photoanodes composited porphyrin‐based compounds. simulation confirm that boosted originates from exceptional rather surface catalysis dynamic. This study provides an efficient strategy tailoring by regulating single‐atom promoting extract boost activity.

Язык: Английский

Процитировано

8