4.6 Article

Inherent Oxygen Vacancies Boost Surface Reconstruction of Ultrathin Ni-Fe Layered-Double-Hydroxides toward Efficient Electrocatalytic Oxygen Evolution

期刊

ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 9, 期 21, 页码 7390-7399

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.1c02256

关键词

oxygen evolution reaction; layered-double-hydroxides; surface reconstruction; oxygen vacancies; p-n interface

资金

  1. National Natural Science Foundation of China [21773093]
  2. Natural Science Foundation of Guangdong Province [2021A1515012351]
  3. China Postdoctoral Science Foundation [2020M673056]

向作者/读者索取更多资源

The ultrathin Ni-Fe layered-double-hydroxides (LDH) with inherent oxygen vacancies (VO) were successfully fabricated via coprecipitation, achieving low overpotential during oxygen evolution reaction (OER) in potassium hydroxide solution. The presence of VO was experimentally and theoretically proven to boost surface reconstruction and enhance OER activity, highlighting the correlation between electrocatalysis and both the catalyst's surface and bulk properties.
Unraveling structure-related reconstruction during oxygen evolution reaction (OER) and its correlation with intrinsic electrocatalytic activity is of great significance for designing better catalysts but unfortunately remains elusive. Herein, ultrathin Ni-Fe layered-double-hydroxides (LDH) with inherent oxygen vacancies (VO) are successfully fabricated via coprecipitation under a controlled manner, which accomplish a quite low overpotential of 230 mV at 10 mA cm(-2) in 1.0 M KOH and perform among the best of recently reported nonprecious electrocatalysts. During the OER, inherent VO is experimentally and theoretically evidenced to boost surface reconstruction and the operando formation of p-n interfaces (i.e., gamma-Ni-Fe LDH/alpha-Ni-Fe LDH) via deprotonation. On such reconstructed interfaces, the VO in both surface gamma-Ni-Fe LDH and bulk alpha-Ni-Fe LDH can alter the electron densities of metal sites and subsequently optimize the free energies of a multistep OER pathway, which accounts for the boosted OER activity and, more importantly, identifies the correlation of electrocatalysis with both the catalyst surface and bulk.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.6
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

Article Chemistry, Multidisciplinary

Recent advances of two-dimensional CoFe layered-double-hydroxides for electrocatalytic water oxidation

Yi Zhou, Jialai Hu, Lichun Yang, Qingsheng Gao

Summary: This review highlights the catalytic performance of earth-abundant CoFe layered-double-hydroxides (LDHs) in the oxygen evolution reaction (OER), focusing on their crystal structure, surface properties, and the role of iron species. Advanced approaches for optimizing the OER activity of CoFe LDHs are comprehensively overviewed, along with an analysis of their unique advantages. Finally, a perspective on the future development of CoFe LDHs electrocatalysts is provided.

CHINESE CHEMICAL LETTERS (2022)

Article Chemistry, Multidisciplinary

Intercalation-Driven Defect-Engineering of MoS2 for Catalytic Transfer Hydrogenation

Yanghao Shi, Wenbiao Zhang, Jingwen Tan, Tianlan Yan, Yingshuai Jia, Zhiyuan Wang, Yi Tang, Qingsheng Gao

Summary: A new route of in situ intercalation is introduced to engineer defects on MoS2, which can be tuned to improve the catalytic performance of the material in the transfer hydrogenation reaction. The intercalation-induced defects enhance the reactivity of MoS2, demonstrating the promise of the defect-engineering strategy for designing TMDs-based catalysts.

ADVANCED MATERIALS INTERFACES (2022)

Article Energy & Fuels

Biomass-Derived Mo2C@N, P Co-Doped Carbon as an Efficient Electrocatalyst for Hydrogen Evolution Reaction

Xing Yin, Junjie Shao, Wenbiao Zhang, Qingsheng Gao

Summary: Cost-efficient electrocatalysts derived from biomass-derived nanomaterials, such as Mo2C@NPC core@shell electrocatalysts obtained from kapok fibers, exhibit high activity for hydrogen evolution reaction (HER) in both acidic and alkaline conditions, as well as satisfactory long-term durability.

ENERGY & FUELS (2022)

Article Chemistry, Physical

Nickel sulfide-oxide heterostructured electrocatalysts: Bi-functionality for overall water splitting and in-situ reconstruction

Zinan Huang, Liuqing He, Wenbiao Zhang, Wenjie Huang, Qijie Mo, Lichun Yang, Qiang Fu, Qingsheng Gao

Summary: By introducing facile O2-plasma activation, bi-functional electrocatalysts with improved performance are constructed via nickel sulfide-oxide heterostructures. The activated Ni3S2-NiOx exhibits lower overpotentials for both HER and OER reactions and a lower voltage for overall water splitting.

JOURNAL OF COLLOID AND INTERFACE SCIENCE (2022)

Article Chemistry, Multidisciplinary

Promoting Amination of Furfural to Furfurylamine by Metal-Support Interactions on Pd/MoO3-x Catalysts

Zhiyuan Wang, Yinjian Zheng, Jiye Feng, Wenbiao Zhang, Qingsheng Gao

Summary: Pd/MoO3-x catalysts were proposed for the reductive amination of furfural, showing high catalytic activity due to the interactions between Pd nanoparticles and MoO3-x supports. The Mo-V-rich MoO3-x acts as an acidic promoter to facilitate carbonyl group activation and also interacts with Pd nanoparticles to promote hydrogenolysis reactions. The efficient Pd/MoO3-x catalyst demonstrates the importance of metal-support interactions in biomass refinery.

CHEMISTRY-A EUROPEAN JOURNAL (2023)

Article Chemistry, Multidisciplinary

Roughness-Dependent Electro-Reductive Coupling of Nitrobenzenes and Aldehydes on Copper Electrodes

Yinjian Zheng, Zhiyuan Wang, Peng Chen, Wenbiao Zhang, Qingsheng Gao

Summary: The electro-reductive coupling of nitro and carbonyl compounds provides a convenient, environmentally friendly and energy benign method for the synthesis of valuable nitrones or imines, but achieving high selectivity remains challenging. In this study, the surface roughness of Cu electrodes is introduced as a determinant to control the switch from nitrones to imines by the controllable reduction of nitroarenes on tailored Cu-I/Cu-0 interfaces. The selectivity of nitrones and imines can be modulated by adjusting the roughness of the Cu electrode, with higher roughness leading to decreased nitrones and increased imines. This surface roughness-dependent selectivity is demonstrated in a wide range of substrates, highlighting the potential of surface engineering for electrochemical synthesis.

CHEMSUSCHEM (2023)

Review Chemistry, Multidisciplinary

Chevrel phases: synthesis, structure, and electrocatalytic applications

Wanling Zhang, Wenbiao Zhang, Jingwen Tan, Yi Tang, Qingsheng Gao

Summary: This review provides an overview of Chevrel phases (CPs) with the chemical formula of MxMo6T8 (T = S, Se, and Te) as noble-metal-free electrocatalysts. It focuses on the representative efforts made and progress achieved in exploring the crystal structure and surface configurations to enhance efficiency. The design, fabrication, and catalytic performance of CPs are discussed in detail, and the potential of CPs in electrocatalysis is highlighted. The review aims to deepen the understanding of CPs and inspire the development of more cost-efficient catalysts.

MATERIALS CHEMISTRY FRONTIERS (2023)

Article Chemistry, Multidisciplinary

Chlorine-mediated electrodeposition of hierarchical and hydrophobic copper electrocatalysts for efficient CO2 electroreduction to ethylene

Yinqiong Wu, Jiye Feng, Danni Shi, Wenbiao Zhang, Yi Tang, Qingsheng Gao

Summary: Hierarchical Cu dendrites fabricated via Cl-mediated electrodeposition exhibit high C2H4 efficiency (58% faradaic efficiency at -0.9 V vs. RHE) for CO2 electroreduction due to their optimal hydrophobicity/aerophilicity and dominant distribution of active (100) and (110) facets.

CHEMICAL COMMUNICATIONS (2023)

Review Chemistry, Physical

Recent progress of Cu-based electrocatalysts for upgrading biomass-derived furanic compounds

Jingwen Tan, Mei Jiang, Kun Yu, Yuyang Song, Wenbiao Zhang, Qingsheng Gao

Summary: The electrochemical upgradation of biomass feedstock is important for achieving carbon cycle without high-grade heat sources. Notably, Cu-based catalysts enable efficient and selective conversion of furanic molecules through electrochemical hydrogenation and oxidation. This review provides insights into the electrochemical processes and discusses the achievements in catalytic performance, mechanism, and electronic efficiency improvement. Future developments in electrocatalysts and electrolysis techniques are also anticipated.

CATALYSIS SCIENCE & TECHNOLOGY (2023)

Article Chemistry, Physical

Alloying promotion of Pd-based metallenes in electrocatalytic hydrogenation of functionalized nitroarenes

Wenbiao Zhang, Wanling Zhang, Jingwen Tan, Di Pan, Yi Tang, Qingsheng Gao

Summary: This study demonstrates the use of two-dimensional Pd-based metallenes as efficient electrocatalysts for the electrocatalytic hydrogenation of nitroarenes, showing the intrinsic promotion of active sites by alloying effects. Among them, a Pd-Mo metallene with a highly exposed active surface and strong electronic interactions between Pd and Mo atoms exhibits high selectivity (>90.0%) and faradaic efficiency (78.3%) for the chemoselective hydrogenation of 4-nitrostyrene (4-NS) to value-added 4-vinylaniline (4-VA), outperforming a homemade Pd metallene and commercial Pd/C.

JOURNAL OF MATERIALS CHEMISTRY A (2023)

Article Chemistry, Multidisciplinary

Promoted electrocatalytic hydrogenation of furfural in a bi-phasic system

Mei Jiang, Jingwen Tan, Yizhong Chen, Wenbiao Zhang, Peng Chen, Yi Tang, Qingsheng Gao

Summary: The promoted electrocatalytic hydrogenation of biomass-derived furfural to 2-methylfuran is identified for the first time in a water/oil bi-phasic system, with the oil phase enabling rapid separation of hydrophobic products from the electrode/electrolyte interfaces, leading to a favorable equilibrium for hydrodeoxygenation.

CHEMICAL COMMUNICATIONS (2023)

Article Nanoscience & Nanotechnology

Activating Commercial Nickel Foam to a Highly Efficient Electrocatalyst for Oxygen Evolution Reaction through a Three-Step Surface Reconstruction

Boxu Gao, Xue Yang, Xueliang Fan, Zhuxin Gui, Wenbiao Zhang, Yingshuai Jia, Sinong Wang, Yahong Zhang, Qingsheng Gao, Yi Tang

Summary: In this research, a three-step preactivation process was proposed to reconstruct commercial nickel foam (CNF) as an efficient electrocatalyst for the oxygen evolution reaction (OER). The activated CNF showed excellent OER performance in alkaline media and could tolerate long-term tests under a large current density. The calcination step led to a reconstructive surface morphology, the high-voltage treatment changed the valence of surface Ni species, and the immersion process introduced Fe heteroatoms into the CNF surface, all contributing to the improved catalytic performance.

ACS APPLIED MATERIALS & INTERFACES (2023)

Article Chemistry, Physical

Enhancing anti-chlorine corrosion of Ni3S2 by Mo-doping for mimic seawater electrolysis

Wanjun Ou, Wenbiao Zhang, Haoran Qin, Weijia Zhou, Yi Tang, Qingsheng Gao

Summary: Introducing Mo-doping enhances the electrocatalytic activity and anti-chlorine corrosion properties of Ni3S2, leading to efficient overall seawater splitting.

JOURNAL OF COLLOID AND INTERFACE SCIENCE (2024)

Article Chemistry, Physical

In situ reconfiguration of plasma-engineered copper electrodes towards efficient electrocatalytic hydrogenation

Peng Chen, Wenbiao Zhang, Jingwen Tan, Yang Yang, Yingshuai Jia, Yi Tang, Qingsheng Gao

Summary: Defect engineering of Cu electrodes via plasma treatment boosts the kinetics of electrocatalytic hydrogenation, enabling the efficient conversion of furfural to furfuryl alcohol. The high Faradaic efficiency of the process is attributed to the quick in situ reduction of CuOx to Cu with rich defects and high roughness.

CATALYSIS SCIENCE & TECHNOLOGY (2022)

暂无数据