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Nanomaterials · 2021 ·Vol. 11 ·期 7 ·1847 · IF 5.076

Highly Enhanced OER Performance by Er-Doped Fe-MOF Nanoarray at Large Current Densities

Yan Ma,Yujie Miao,Guomei Mu,Dunmin Lin,Chenggang Xu,Wen Zeng,Fengyu Xie

Great expectations have been held for the electrochemical splitting of water for producing hydrogen as a significant carbon-neutral technology aimed at solving the global energy crisis and greenhouse gas issues. However, the oxygen evolution reaction (OER) process must be energetically catalyzed over a long period at high output, leading to challenges for efficient and stable processing of electrodes for practical purposes. Here, we first prepared Fe-MOF nanosheet arrays on nickel foam via rare-earth erbium doping (Er0.4Fe-MOF/NF) and applied them as OER electrocatalysts. The Er0.4Fe-MOF/NF exhibited wonderful OER performance and could yield a 100 mA cm−2current density at an overpotential of 248 mV with outstanding long-term electrochemical durability for at least 100 h. At large current densities of 500 and 1000 mA cm−2, overpotentials of only 297 mV and 326 mV were achieved, respectively, revealing its potential in industrial applications. The enhancement was attributed to the synergistic effects of the Fe and Er sites, with Er playing a supporting role in the engineering of the electronic states of the Fe sites to endow them with enhanced OER activity. Such a strategy of engineering the OER activity of Fe-MOF via rare-earth ion doping paves a new avenue to design other MOF catalysts for industrial OER applications.Keywords:rare-earth doping;MOFs;large current;electronic structure

研究领域: 材料科学 · 电化学
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Inorganic Chemistry Frontiers · 2023 ·Vol. 11 ·期 4 ·1153-1166 · IF 7

Construction of a phosphorus-based integrated electrode for efficient and durable seawater splitting at a large current density

Jiajing Xia,Lujia Zhang,Yizhou Wang,Weiju Hao

Constructing economical and corrosion-resistant catalytic electrodes for efficient and high-current seawater splitting is a significant challenge. Herein, we employed a gentle, one-step immersion method to obtain an efficient and stable self-supporting integrated catalytic electrode via nickel foam (NF) etched in situ by sodium hypophosphite and trace ruthenium (Ru@P–NF). The successful growth of spherical Ru on the P–NF resulted in high intrinsic activity and rapid electron transfer capabilities. The Ru@P–NF electrode achieved a current density of 100 mA cm−2 in the hydrogen evolution reaction (HER) with an overpotential of only 32 mV in an alkaline simulated seawater system (1 M KOH + 0.5 M NaCl). An overpotential of only 153 mV resulted in a current density of 10 mA cm−2 in the oxygen evolution reaction (OER). Moreover, this electrode necessitated a mere 1.42 V at 20 mA cm−2 to facilitate overall water splitting. Impressively, the operation of Ru@P–NF was stable at 100 mA cm−2 for over 1500 hours without significant degradation, and thus demonstrated stable catalysis for an impressive 300 h at an industrial-level high current density in a weakly alkaline seawater and urine system. This work provides robust theoretical support for the construction of efficient industrial-scale catalytic electrodes for water electrolysis.

CAS / MDL: 12030-49-8
研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

In situ synthesis of two-dimensional graphene-like nickel-molybdenum nitride as efficient electrocatalyst towards water-splitting under large-current density

Yibing Liu,Bowen Zhou,Yubing Zhang,Weiping Xiao,Bin Li,Zexing Wu,Lei Wang

Transition metal nitride (TMNs) electrocatalysts have attracted tremendous attentions for their unique electron structure, high activity, and excellent stability. Herein, a two-dimensional (2D) graphene-like structured nickel-molybdenum nitride (Ni-MoN) on nickel foam (NF), is prepared via facile hydrothermal and following nitridation process. The as-prepared Ni-MoN-450 (pyrolysis at 450 °C) displays good hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performances in alkaline media. Only 22 mV and 117 mV are needed to achieve current densities of 10 mA cm −2 and 500 mA cm −2 in 1.0 M KOH, respectively, toward HER. The assembled two-electrode system, with the synthesized Ni-MoN-450 as the anode and cathode, exhibits good performance to achieve 1000 mA cm −2 in 1.0 M KOH + 25 °C and 6.0 M KOH + 80 °C. Moreover, it also presents long-term stability under large-current density, which verified its robust property.

研究领域: 材料科学 · 电化学
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CHEMISTRY-A EUROPEAN JOURNAL · 2023 ·Vol. 29 ·期 56 ·e202301521 · IF 4.3

Synergistic Promotion of Large-Current Water Splitting through Interfacial Engineering of Hierarchically Structured CoP−FeP Nanosheets with Rich P Vacancies

Luoluo Qi,Zhiyang Huang,Miao Liao,Lei Wang,Lixia Wang,Mingcheng Gao,Tayirjan Taylor Isimjan,Xiulin Yang

Graphical A CoP−FeP heterostructure catalyst with abundant P vacancies (Vp−CoP−FeP/NF) on nickel foam is constructed through impregnation and phosphorization. It demonstrates excellent hydrogen evolution performance and has practical application prospects in high-current overall water splitting. The catalyst‘s unique hierarchical nanosheet structure, plentiful P vacancies and synergistic effect of CoP and FeP accelerate HER kinetics, resulting in its superior performance. The development of hydrogen evolution reaction (HER) catalysts with high performance under large current density is still a challenge. Introducing P vacancies in heterostructure is an appealing strategy to enhance HER kinetics. This study investigates a CoP−FeP heterostructure catalyst with abundant P vacancies (Vp−CoP−FeP/NF) on nickel foam (NF), which was prepared using dipping and phosphating treatment. The optimized Vp−CoP−FeP catalyst exerted prominent HER catalytic capability, requiring an ultra-low overpotential (58 mV @ 10 mA cm −2 ) and displaying robust durability (50 h @ 200 mA cm −2 ) in 1.0 M KOH solution. Furthermore, the catalyst demonstrated superior overall water splitting activity as cathode, demanding only cell voltage of 1.76 V at 200 mA cm −2 , outperforming Pt/C/NF (−) || RuO 2 /NF (+) . The catalyst‘s outstanding performance can be attributed to the hierarchical structure of porous nanosheets, abundant P vacancies, and synergistic effect between CoP and FeP components, which promote water dissociation and H* adsorption and desorption, thereby synergically accelerating HER kinetics and enhancing HER activity. This study demonstrates the potential of HER catalysts with phosphorus-rich vacancies that can work under industrial-scale current density, highlighting the importance of developing durable and efficient catalysts for hydrogen production.

研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

B-doping-induced amorphization of LDH for large-current-density hydrogen evolution reaction

Hongyuan Yang,Ziliang Chen,Peifang Guo,Ben Fei,Renbing Wu

Developing a platinum-free hydrogen evolution reaction (HER) electrocatalyst that can steadily drive a large current density is of great significance in a commercially electrochemical water splitting technology. Herein, we show that the B-doping-induced amorphization of crystalline layered double hydroxide (LDH) activates it as an extremely efficient HER catalyst. The amorphous B-incorporated nickel-cobalt LDH supported on the nickel foam (A-NiCo LDH/NF) can yield large current densities at small overpotentials (100 mA cm –2 at 151 mV, 500 mA cm –2 at 286 mV, and 1000 mA cm –2 at 381 mV) with high durability in alkaline medium even after 72 h, which is even better than commercial platinum. This work may provide a promising way for structure tuning of transition metal LDH to effectively boost HER efficiency towards practical water electrolysis.

研究领域: 材料科学 · 电化学
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Chemistry-An Asian Journal · 2020 ·Vol. 15 ·期 9 ·1484-1492 · IF 4.056

Synergistic Assembly of a CoS@NiFe/Ni Foam Heterostructure Electrocatalyst for Efficient Water Oxidation Catalysis at Large Current Densities

Muheng Wang,Yun Wu,Na Li,Fei Zhao,Qiang Zhao,Jinping Li,Guang Liu

Graphical Benefiting from synergistic effects between a NiFe layer and CoS film, the obtained heterostructure CoS@NiFe/NF electrocatalyst displayed excellent oxygen evolution reaction activities at high current densities towards water splitting. Electrochemical water splitting is an ideal pollution-free path to generate hydrogen at large scale, however, the development of highly catalytic electrocatalysts for the water oxidation reaction at large current densities is still a fundamental challenge. Herein, we report a novel, high-wettability water-oxidation electrocatalyst composed of an amorphous NiFe layer and CoS film on commercial nickel foam via a two-step electrodeposition synthetic path. Benefiting from the strong interactions between the NiFe layer and CoS film, enlarged surface active sites and enhanced wettability, the CoS@NiFe/NF electrode exhibited an outstanding water oxidation performance at 10 mA/cm 2 with an overpotential of 175 mV in 1 M KOH solution and steadily delivered a current density of 1 A/cm 2 at merely 330 mV in 30 wt% KOH solution. Even at large densities, the CoS@NiFe/NF hybrids also showed excellent water oxidation stability and corrosion resistance for at least 24 h. Such a synergistic assembling approach to fabricate a CoS@NiFe/NF heterostructure together with excellent OER performance may be a promising strategy for rationally building and designing heterostructural electrocatalysts towards highly efficient water oxidation reaction.

CAS / MDL: 10026-22-9 1310-58-3
研究领域: 材料科学 · 电化学
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ACS Sustainable Chemistry & Engineering · 2021 · IF 8.198

Dual Modification Strategy of Nickel Sulfide as pH-Universal Catalysts for Hydrogen Production at Large Current Density

Yun Tong,Dongmei Feng,Pengzuo Chen

Developing highly efficient electrocatalysts for large-scale implementation of the hydrogen evolution reaction (HER) at a large current density is critical for renewable H2 fuel. The designed electrocatalysts by non-noble metals are expected to operate well at wide pH conditions, but it remains a major challenge. In this work, a novel dual modification strategy is applied to develop a series of P/Mo modified Ni3S2 on nickel foam (denoted as P-MNS/NF) as pH-universal electrocatalysts for HER. Benefiting from the plentiful catalytic active sites, optimized electronic structure, and improved reaction kinetics, the P-MNS/NF electrode realizes remarkable catalytic activity and stability at a large current density. The optimal P3-MNS3/NF catalyst exhibits the low overpotential of 245 and 243 mV at a high current density of 1 A cm–2 for both alkaline/acidic media. Those are promising performance results compared to those of the other nickel sulfide-based materials. Importantly, this P3-MNS3/NF can also achieve good performance in a neutral electrolyte. This needs a small overpotential of 360 mV to reach the current density of 0.5 A cm–2. Our strategy provides a new method to guide rational design of highly active HER electrocatalysts over a wide pH window.

CAS / MDL: 62-56-6
研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

3D porous network heterostructure NiCe@NiFe electrocatalyst for efficient oxygen evolution reaction at large current densities

Guang Liu,Muheng Wang,Yun Wu,Na Li,Fei Zhao,Qiang Zhao,Jinping Li

Three-dimensional (3D) self-supporting porous network NiCeO x @NiFeO x electrocatalyst on Ni foam (denotes as NiCe@NiFe/NF-N) is prepared by a simple two step electrodepositing process. NiCe@NiFe/NF-N attains 100 mA/cm 2 at overpotential of 254 mV with Tafel slope of 59.9 mV/dec, which is much lower than that of NiCe@NiFe/NF-P, NiFe@NF, NiCe@NF and also commercial RuO 2 electrocatalysts. Furthermore, the obtained NiCe@NiFe/NF-N electrocatalyst only needs overpotential of 359 mV to deliver high current densities of 1 A/cm 2 and demonstrates excellent stability at such large current densities for 20 h, which is also superior to that of NiCe@NiFe/NF-P electrocatalyst. Further study reveals that the enhanced water oxidation performance of NiCe@NiFe/NF-N electrocatalyst with good stability at high current densities could be attributed to the optimal surface and electronic structures, fast reaction kinetics and high intrinsic catalytic activity. Collectively, such electrocatalyst paves new opportunities for development of low-cost water oxidation electrocatalysts with high current densities for practical water splitting applications.

CAS / MDL: 10294-41-4 1310-58-3
研究领域: 材料科学 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Amorphous/crystalline NiFe LDH hierarchical nanostructure for large-current-density electrocatalytic water oxidation

Yilong Li,Mingzhe Li,Chenxuan Xie,Ziyu Ling,Yuzhen Lv,Kepi Chen

Amorphous structure shows more catalytic active sites but poor conductivity towards oxygen evolution reaction (OER). Herein, we fabricated a novel three-dimensional (3D) self-supported NiFe layered double hydroxides (LDH) catalytic material with amorphous/ crystalline interface, aiming to obtain both excellent catalytic activity and conductivity. This homogeneous hierarchical structure exhibits a high catalytic activity and robustness, giving the industrially required current density of 1000 mA cm −2 at an ultralow overpotential of 359.8 mV with 240-hour stability in 1 M KOH. In-situ electrochemical tests reveal that the amorphous/crystalline interface boosts the intermediates evolution and OER kinetics, which might be ascribed to considerable active sites and fast charge transfer. Moreover, the 3D structure has unique superhydrophilicity and superaerophobicity, which can further accelerate the electrolyte penetration, facilitate the bubbles desorption from the electrode, enhance mass transport, and thus improve OER performance at large current densities. This work provides a feasible way to develop high-performance electrocatalytic material via constructing homogeneous amorphous/crystalline interface.

研究领域: 材料科学 · 电化学
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Small · 2021 ·Vol. 18 ·期 2 ·2103866 · IF 13.281

Directionally In Situ Self-Assembled, High-Density, Macropore-Oriented, CoP-Impregnated, 3D Hierarchical Porous Carbon Sheet Nanostructure for Superior Electrocatalysis in the Hydrogen Evolution Reaction

Xiaoyan Wang,Yang Fei,Jie Chen,Yixiang Pan,Weiyong Yuan,Lian Ying Zhang,Chun Xian Guo,Chang Ming Li

3D ZIF-67-particles-impregnated cellulose-nanofiber nanosheets with oriented macropores are synthesized via directional-freezing-assisted in situ self-assembly, and converted to 3D CoP-nanoparticle (NP)-embedded hierarchical, but macropores-oriented, N-doped carbon nanosheets via calcination and phosphidation. The obtained nanoarchitecture delivers overpotentials at 10 and 50 mA cm −2 and Tafel slope of 82.1 and 113.4 mV and 40.8 mV dec −1 in 0.5 M H 2 SO 4 , and of 97.1 and 136.6 mV and 51.2 mV dec −1 in 1 M KOH, all of which are superior to those of the most reported non-noble-metal-based hydrogen evolution reaction (HER) catalysts. This catalyst even surpasses commercial Pt/C for a much lower overpotential at high current densities, which is essential for large-scale hydrogen production. Its catalytic activity can be further optimized to become one of the best in both 0.5 M H 2 SO 4 and 1 M KOH. The outstanding catalytic activity is ascribed to the uniformly-dispersed small CoP NPs in the 3D carbon sheets and the hierarchical nanostructure with rich oriented pores. This work develops a facile, economical, and universal self-assembly strategy to fabricate uniquely nanostructured hybrids to simultaneously promote charge transfer and mass transport, and also offers an inexpensive and high-performance HER catalyst toward industry-scale water splitting.

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2022 · IF 7.336

Constructing sulfide/phosphide heterostructure boosts the activity of iron-manganese bimetallic electrocatalysts for oxygen evolution reaction at large current densities

Jinwei Wang,Yijie Zhang,Weiyi Zhang,Qiang Zhao,Jinping Li,Guang Liu

Designing earth-abundant electrocatalysts with high activity and stability is crucial to the industrial large-scale water splitting for hydrogen production. Herein, we report an effective electrocatalyst composed of inner FeMnP layer and outer FeMnS species for oxygen evolution reaction (OER). The interfacial coupling between two layers modulates the local electronic structure, reduces the indirect contact resistance, optimizes the kinetics of OER, and ultimately boosts the intrinsic OER activity. Meanwhile, the outer FeMnS nanoflowers composed of numerous nanosheets lead to a larger electrochemical surface area (ECSA), exposing more active sites, which also plays a major role in the improvement of ability to catalyze water oxidation. More importantly, the electrode has a hydrophilic/underwater aerophobic surface to insure electrolyte diffusion efficiently and the bubbles release rapidly at a large current density of OER. Therefore, the obtained FeMnS/FeMnP/NF can output the current density of 1000 mA/cm 2 with a low overpotential of 374 mV and can remain such a high current density for over 60 h. It also presents remarkable activity and stability in 30 wt% KOH solution and simulated seawater. This work presents a promising strategy for preparing high-efficiency and low-cost self-supporting electrodes for water oxidation.

研究领域: 材料科学 · 电化学
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Small Methods · 2025 · IF 9.1

Ag on NiCo Layered Double Hydroxide as Oxygen Evolution Electrocatalyst for Anion Exchange Membrane Water Electrolyzer Under Large Current Densities

Yan Sun,Gongjin Chen,Fatima El bachraoui,Yingdan Cui,Guimei Liu,Fei Xiao,Xitang Qian,Zhiwen Xu,Minhua Shao

A facile and universal strategy is employed to synthesize Ag decorated NiCo layered double hydroxide (LDH) heterogeneous structure for the oxygen evolution reaction (OER). The Ag nanoparticles are deposited on NiCo LDH nanosheets via a spontaneous redox reaction. The synthesized Ag/NiCo LDH achieves an overpotential of 460 mV at a current density of 1 A cm −2 geo , surpassing that of NiCo LDH (722 mV). In an anion exchange membrane water electrolyzer (AEMWE) with Ag/NiCo LDH as the anode and Pt/C as the cathode, the cell can deliver an ultrahigh current density of 5 A cm −2 at a low voltage of 2.10 V. This superior current density is nearly four times larger than that of AEMWEs with other non-precious anode electrocatalysts reported in literature under the same effective area. Furthermore, it exhibits desired durability with no performance decay for over 300 h at 1 A cm −2 , which is almost six times longer than that of electrolyzer with an IrO 2 anode. Operando electrochemical impedance spectroscopy results reveal that Ag decoration facilitates active site formation and reduces the OER onset potential compared to NiCo LDH. This study showcases a practical approach to designing highly effective and durable OER electrocatalysts in industrial hydrogen production.

研究领域: 材料科学 · 电化学
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