JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Meijia Liu,Lin Wu,Yafeng Li,Shuai Chen,Yuhang Lei,Zhuang Huo,Lin Tao,Lixiang Li,Chengguo Sun,Han Zhang,Baigang An
Non-precious metals with tailored phase structures show promise as oxygen evolution reaction (OER) catalysts due to their high inherent catalytic activity and extensive exposed active surface area. However, the mechanisms by which phase structures enhance catalytic performance remain unclear. Herein, we synthesized an amorphous cobalt boride (CoB) catalyst via a magnetic field-assisted method, yielding uniform nanoparticles that self-assemble into a nanobead structure. This material undergoes heat treatment to transition from an amorphous phase to a crystalline phase. The catalyst demonstrated exceptional OER activity and long-term stability in an alkaline electrolyte, requiring only 350 mV overpotential at 10 mA cm −2 . The amorphous CoB demonstrates remarkable durability by maintaining stable operation for 100 h under harsh conditions characterized by high alkalinity and elevated temperature without any observable performance degradation. We demonstrate that electrochemical activation of an amorphous catalyst can unveil active sites within the bulk material, leveraging the short-range order characteristic of amorphous structures. This process significantly amplifies the active site density, consequently enhancing the electrocatalytic performance of the amorphous catalyst in the oxygen evolution reaction within water oxidation. Furthermore, in situ Raman spectroscopy reveals that amorphous CoB rapid self-reconstruction upon electrochemical activation, leading to the formation of a metal (oxy)hydroxide active layer. This study offers valuable insights into the design of high-efficiency OER catalysts by elucidating the mechanisms underlying amorphous and crystalline materials.
研究领域:
材料科学
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电化学
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能源转换
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yanyan Wu,Ying Li,Mengke Yuan,Hongru Hao,Xiaojiao San,Zhe Lv,Lingling Xu,Bo Wei
Earth-abundant catalysts for both Oxygen evolution reaction (OER) and Hydrogen evolution reaction (HER) are highly required for electrochemical water splitting. Transition metal sulfides have been considered as efficient catalysts for both OER and HER, but their real active species in operation condition are still controversial. Herein, self-supported Ni 3 S 2 /FeNi 2 S 4 nanosheets (Ni-Fe-S) are synthesized and in-situ Raman measurement is conducted to monitor the phase transformation under realistic conditions. Combined with a series of ex-situ technologies , it can be concluded that, Ni-Fe-S nanosheets function as pre-catalysts which undergo dynamically structural reconstruction during electrolysis. The active species are determined to be γ-NiOOH for OER and metallic Ni 0 for HER in 1 M KOH media, respectively. As-converted products only need overpotentials of 50 mV for HER and 201 mV for OER to achieve the current density of 10 mA cm - 2 , respectively. A two-electrode electrolyzer can afford a current density of 10 mA cm - 2 at a low cell voltage of 1.55 V. This work provides new perspectives to recognize the catalytic evolution process of nickel-based sulfides for water splitting and sheds light on the rational design of bifunctional materials in energy devices.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Nature Communications
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2025
·Vol. 16
·期 1
·1-11
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IF 15.7
Quan Quan,Zhang Yuxuan,Li Haifan,Wang Wei,Xie Pengshan,Chen Dong,Wang Weijun,Meng You,Yin Di,Li Yezhan,Song Dongyuan,Chen Lijie,Li Shaohai,Yang Cheng,Yanagida Takeshi,Wong Chun-Yuen,Yip SenPo,Ho Johnny C.
Maximizing metal-substrate interactions by self-reconstruction of coadjutant metastable phases can be a delicate strategy to obtain robust and efficient high-density single-atom catalysts. Here, we prepare high-density iridium atoms embedded ultrathin CoCeOOH nanosheets (CoCe-O-Ir SA ) by the electrochemistry-initiated synchronous evolution between metastable iridium intermediates and symmetry-breaking CoCe(OH) 2 substrates. The CoCe-O-Ir SA delivers an overpotential of 187 mV at 100 mA cm −2 and a steady lifespan of 1000 h at 500 mA cm −2 for oxygen evolution reaction. Furthermore, the CoCe-O-Ir SA is applied as a robust anode in an anion-exchange-membrane water electrolysis cell for seawater splitting at 500 mA cm −2 for 150 h. Operando experimental and theoretical calculation results demonstrate that the reconstructed thermodynamically stable iridium single atoms act as highly active sites by regulating charge redistribution with strongly p - d - f orbital couplings, enabling electron transfer facilitated, the adsorption energies of intermediates optimized, and the surface reactivity of Co/Ce sites activated, leading to high oxygen evolution performance. These results open up an approach for engineering metastable phases to realize stable single-atom systems under ambient conditions toward efficient energy-conversion applications.
研究领域:
材料科学
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电化学
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催化科学
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Chaoran Pi,Difei Leng,Xuming Zhang,Shuangjie Wu,Yun Li,Li Huang,Zhihong Liu,Paul K. Chu,Kaifu Huo
The self-reconstruction of electrocatalysts during the cathodic hydrogen evolution reaction (HER) has garnered significant interest due to its impact on microstructure and electrocatalytic efficiency. Understanding the mechanisms driving this transformation is crucial for the development of high-performance HER pre-catalysts. In this study, an efficient Co(OH) 2 (001)/MoN (002) heterostructured catalyst is fabricated through the self-reconstruction of the Co/MoN pre-catalyst and the mechanism of facet-induced reconstruction is investigated in detail. This Co/MoN pre-catalyst exhibits an impressive 58 % reduction in overpotential at a constant current density of 100 mA cm −2 over 5 h. It ultimately achieves a low overpotential of 339 mV at 1 A cm −2 , outperforming commercial Pt/C under similar current conditions, while maintaining high current activity with 99.4 % retention after 110 h of continuous electrolysis. Operando characterizations and theoretical simulations reveal that metallic Co dissolves rapidly under bias as H + ions infiltrate the interstitial spaces, and the dissolved Co 2+ ions preferentially deposit as Co(OH) 2 nanosheets. This deposition aligns with the (001) facet of Co(OH) 2 and the prominent (002) plane of the MoN matrix through lattice matching, exhibiting a very low interfacial formation energy. Density-functional theory analysis reveals that the alignment of the crystal facets between Co(OH) 2 (001) and MoN (002) enhances electron transfer and modulates the interface to boost the water dissociation and hydrogen adsorption activity and kinetics. Our results underscore the importance of precise control over the reconstruction process for cathodic HER and facilitate the development of advanced transition metal-based electrocatalysts for industrial alkaline hydrogen production.
研究领域:
材料科学
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电化学
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理论计算
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Shenghua Ye,Yaqi Lei,Tingting Xu,Lirong Zheng,Zhida Chen,Xiuyuan Yang,Xiangzhong Ren,Yongliang Li,Qianling Zhang,Jianhong Liu
In this study, phosphate FeCo(H 3 O)(PO 4 ) 2 nanosheet arrays (NAs) were synthesized using an electrochemical strategy. FeCo(H 3 O)(PO 4 ) 2 NAs as precatalyst could undergo significant self-reconstruction, including leaching of phosphate anions and electro-oxidation of Co 2+ during anodizing at the potential range of oxygen evolution reaction (OER) in 1 M KOH solution, eventually resulting in the formation of Fe 0.5 Co 0.5 OOH NAs with low crystallinity . The high content of Fe in Fe 0.5 Co 0.5 OOH NAs promoted the formation of active Fe 3+ –O–Fe 3+ motifs that increased OER occurrence. Additionally, Fe incorporation increased the ratio of the reaction rate constants of oxygen evolution to Co 3+ /Co 4+ (k OER /k M,ox ) and enhanced the reaction order on the hydroxyl ion . These factors significantly contributed to the outstanding OER catalytic performances of Fe 0.5 Co 0.5 OOH NAs.
研究领域:
材料科学
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电化学
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DOI
高影响因子
ChemCatChem
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2024
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IF 3.8
Chao Wang,Chunqun Qin,Mingzheng Liao,Yanping Du,Jiming Gao,Yanbing Wu
High-entropy oxides (HEOs), known for their excellent thermodynamic stability due to their high-entropy effect. In this study, high-entropy (NixAlCoCrMn)3O4 oxides of spinel structure were synthesized by sol-gel method. This HEO has a self-reconfiguration properties in the reaction, and its internal Ni and Co ions exsolve to form a uniformly dispersed NiCot alloy on the surface. The increase of Ni content promotes the exsolution of Ni and Co ions from the interior of the spinel. The high-entropy with a large number of oxygen vacancies not only possesses a stable structure to limit the migration of NiCo alloys, but also enhances the hydrogen overflow. In the CO methanation reaction, it has 99% CO conversion with 87% methane selectivity within 400 oC, and it is stable in the long-term test. This work provides a new idea for exploring the use of high-entropy materials to improve thermal catalytic activity and stability.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Wei Wang,Yunlei Zhong,Xinyu Zhang,Sainan Zhu,Yourong Tao,Yanxin Zhang,Hongsen Zhu,Yifei Zhang,Xingcai Wu,Guo Hong
Surface self-reconstruction by the electrochemical activation is considered as an effective strategy to increase the oxygen evolution reaction (OER) performance of transition metal compounds. Herein, uniform Co 2 (OH) 3 Cl microspheres are developed and present an activation-enhanced OER performance caused by the etching of lattice Cl − after 500 cyclic voltammetry (CV) cycles. Furthermore, the OER activity of Co 2 (OH) 3 Cl can be further enhanced after small amounts of Fe modification (Fe 2+ as precursor). Fe doping into Co 2 (OH) 3 Cl lattices can make the etching of surface lattice Cl − easier and generate more surface vacancies to absorb oxygen species. Meanwhile, small amounts of Fe modification can result in a moderate surface oxygen adsorption affinity, facilitating the activation of intermediate oxygen species. Consequently, the 10% Fe-Co 2 (OH) 3 Cl exhibits a superior OER activity with a lower overpotential of 273 mV at 10 mA cm −2 (after 500 CV cycles) along with an excellent stability as compared with commercial RuO 2 .
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
ACS Nano
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2018
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IF 13.709
Yecan Pi,Qi Shao,Xing Zhu,Xiaoqing Huang
The anodic oxygen evolution reaction (OER) is central to various energy conversion devices, but the investigation of the dynamic evolution of catalysts in different OER conditions remains quite limited, which is unfavorable for the understanding of the actual structure–activity relationship and catalyst optimization. Herein, we constructed monodispersed IrNix nanoparticles (NPs) with distinct composition-segregated features and captured their structural evolution in various OER environments. We decoded the interesting self-reconstruction of IrNix NPs during the OER, in which an Ir-skin framework is generated in an acidic electrolyte, while a Ni-rich surface layer is observed in an alkaline electrolyte owing to Ni migration. Benefiting from such self-reconstruction, considerable OER enhancements are achieved under both acidic and alkaline conditions. For comparison, IrNix nanoframes with Ir skins prepared by chemical etching show a similar structural evolution result in the acidic electrolyte, but a total different phenomenon in the alkaline electrolyte. By tracking the structural evolution of IrNix catalysts and correlating them with OER activity trajectories, the present work provides a significant understanding for designing efficient OER catalysts with controlled compositional distributions.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
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2023
·Vol. 10
·期 12
·3621-3631
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IF 7
Fanan Wang,Lianggao Hu,Renzhi Deng,Shiwei Dai,Dongfei Lu,Xin Chen,Xinchen Pan,Xinyi Ren,Dibo Dong,Rengui Weng,Gang Xu,Hongbin Yang
The self-reconstruction of Ni-based electrodes and the in situ generation of oxy-hydroxides are widely investigated as crucial prerequisites for efficient oxygen evolution reaction (OER). However, the transformation is usually time-consuming and surface-limited, resulting in insufficient active sites with unsatisfactory intrinsic activity. Herein, we provide a NH3-treated Fe-doped NiMoO4 hydrate as a highly active OER pre-catalyst, with an overpotential of only 240 mV at 100 mA cm−2 and 270 mV at 300 mA cm−2. By combination of multiple quasi-situ and in situ techniques, the enhanced performance is ascribed to the lattice distortion in the pre-catalyst induced by the NH3 treatment. Firstly, the lattice defects with tensile strain and voids accelerate the selective dissolution of MoO42− and ensure the rapid and bulk reconstruction of the pre-catalyst with enriched active sites. Moreover, it could modulate the electronic structure and optimize the synergism between Ni and Fe, facilitating the dynamic evolution of Fe-doped γ-NiOOH (γ-Ni(Fe)OOH). The intimately interacted Ni–Fe dual-sites from γ-Ni(Fe)OOH and the resultant distorted structure facilitate the formation and adsorption of active oxygen species, accounting for the improved intrinsic activity for OER.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Nanoscale
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2025
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IF 5.1
Lili Guo,Yanan Huang,Yue Qin,Bin Chen,Chang Liu,Hao Chen,Junfeng Zhang,Xiangwen Zhang,Qingfa Wang
Anion exchange membrane water electrolysis (AEMWE) is a promising advanced strategy for large-scale green hydrogen production. Developing highly active, stable, and low-cost oxygen evolution reaction materials is still challenging. Herein, a core–shell FeCoNiMoW@FeCoNiOOH electrocatalyst was fabricated by in situ self-reconstruction of FeCoNiMoW high entropy alloy prepared via the fast carbothermal shock method. The surface Mo and W as sacrificing agents were etched in the reconstruction of the catalyst to generate more oxygen vacancies and form the FeCoNiOOH-rich medium entropy alloy shell, which is enriched in more active species M-OOH (i.e., NiOOH, CoOOH, FeOOH) to promote the OH adsorption. The medium/high entropy core–shell structure derived from self-reconstruction exhibited not only high activity but also excellent corrosion resistance, evidenced by an overpotential of 246 mV at 10 mA cm−2 and a robust stability of 1000 h at 100 mA cm−2. Moreover, this core–shell FeCoNiMoW@FeCoNiOOH-based anion exchange membrane water electrolyzer demonstrated a low cell voltage of 1.74 V to achieve a practical current density of 1 A cm−2 and exhibited remarkable stability for 430 h with a decay rate of only 0.023 mV h−1. This work provides guidance on designing cost-effective and outstanding corrosion-resistant OER electrocatalysts for anion exchange membrane water electrolysis.
研究领域:
材料科学
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电化学
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能源技术
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DOI
PubMed
高影响因子
Energy & Environmental Science
·
2018
·Vol. 11
·期 10
·2945-2953
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IF 30.067
Sanzhao Song,Jing Zhou,Xiaozhi Su,Yu Wang,Jiong Li,Linjuan Zhang,Guoping Xiao,Chengzhi Guan,Renduo Liu,Shuguang Chen,Hong-Ji Lin,Shuo Zhang,Jian-Qiang Wang
Exploring high-performance electrocatalysts for the oxygen evolution reaction (OER) is pivotal for renewable energy storage and conversion. The surface self-reconstruction during the OER is considered as the key of highly active catalysts, whereas identifying the local electronic and geometric structure of the reconstruction-derived components is challenging. Herein, an in situ exsolution method towards the typical LaCo0.8Fe0.2O3−δ perovskite is developed to obtain a new type of lanthana-anchored CoFe catalyst. The optimized catalyst exhibits a low overpotential of 293 mV to reach the current density of 10 mA cm−2 in 0.1 M KOH. Most importantly, operando X-ray absorption spectroscopy (XAS) measurements demonstrate that the CoFe species in the catalyst are nearly transformed into unique (Co/Fe)O(OH) with a definite coordination-unsaturated structure under electrochemical conditions, which actually contributes to this superior performance. Moreover, the presence of the lanthana support promotes this transformation. Our work not only suggests a facile reconstructive strategy to dramatically enhance the OER activity of perovskite oxides in alkaline media, but also unravels the fine structure of true active sites through operando X-ray spectroscopic tracking.
研究领域:
材料科学
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催化化学
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能源存储与转换
✓ 已验证
DOI
高影响因子
Advanced Science
·
2020
·Vol. 7
·期 5
·1902830
·
IF 15.84
Ruchun Li,Bihua Hu,Tongwen Yu,Haixin Chen,Yi Wang,Shuqin Song
Rational design of unique pre-catalysts for highly active catalysts toward catalyzing the oxygen evolution reaction (OER) is a great challenge. Herein, a Co-derived pre-catalyst that allows gradual exposure of CoOOH that acts as the active center for OER catalysis is obtained by both phosphate ion surface functionalization and Mo inner doping. The obtained catalyst reveals an excellent OER activity with a low overpotential of 265 mV at a current density of 10 mA cm −2 and good durability in alkaline electrolyte, which is comparable to the majority of Co-based OER catalysts. Specifically, the surface functionalization produces lots of Co-PO 4 species with oxygen vacancies which can trigger the surface self-reconstruction of pre-catalyst for a favorable OER reaction. Density functional theory calculations reveal that the Mo doping optimizes adsorption-free energy of *OOH formation and thus accelerates intrinsic electrocatalytic activity. Expanding on these explorations, a series of transition metal oxide pre-catalysts are obtained using this general design strategy. The work offers a fundamental understanding toward the correlation among surface-structure-activity for the pre-catalyst design.
研究领域:
材料科学
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电催化
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）