CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Tian Meng,Qun Li,Mengxia Yan,Dewen Wang,Libing Fan,Xiaojuan Liu,Zhicai Xing,Xiurong Yang
Self-reconstruction of oxygen evolution reaction (OER) catalyst, especially metal (oxy)hydroxides or oxides, has attracted much attention. Herein, an in-situ self-reconstruction process for Ni, Fe, Zn ternary-metal hydroxides (NFZ-TH) involving significant morphology transformation, and self-modulated electronic structure change of Ni and Fe owing to the etching of Zn species under anodic polarization potential is revealed. NFZ-TH derived materials, undergoing in-situ self-reconstruction (NFZ-TH-SR), exhibits superior OER performance (η = 217 mV @ j = 10 mA cm −2 geometry ) and excellent stability over a period of ~48 h. Nano-pitted surface resulting from etching of Zn species improves the electrochemical surface area. Meanwhile, in NFZ-TH-SR, large amounts of defects induced defect-/corner-sited Fe and adjustability of NiOOH species are verified by Mössbauer spectra and in-situ Raman spectra respectively. Density functional theory calculations give insight that both defect-/corner- sited Fe and Ni at next-nearest-neighbour defect-site have high activity. This paper helps understand that the proposed in-situ self-reconstruction strategy can improve the electrochemical performance of OER catalysts.
研究领域:
电化学
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材料科学
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催化
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表面科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Huibing Liu,Xinchen Xu,Haoxiang Xu,Shitao Wang,Ziqiang Niu,Qiaohuan Jia,Liu Yang,Rui Cao,Lirong Zheng,Dapeng Cao
The high voltage in oxygen evolution reaction (OER) often causes structural change in electrocatalysts and forms multiple active sites. Therefore, exploring the synergy of various active sites is extremely significant to develop catalysts for OER with multiple elementary steps. Herein, we adopt the physically adsorbed metal ions method to successfully synthesize a highly-efficient electrocatalyst containing the dual active sites of Fe-NiOOH and NiC 4 single atoms (marked as Ni SAs/Fe-NiOOH). The Ni SAs/Fe-NiOOH displays outstanding OER performance with an overpotential of 269 mV to deliver current density of 10 mA/cm 2 that shows 55 mV superior to commercial IrO 2 /CB at the same condition. Experiments and density functional theory calculations indicate that the excellent OER activity of Ni SAs/Fe-NiOOH catalyst is attributed to the synergy of dual active sites of NiC 4 SAs and Fe-NiOOH. A tandem catalysis mechanism is also proposed to reveal the synergism of two active centers, which makes the potential-determining step more facile and accordingly decreases the OER overpotential. This work offers a new concept of tandem catalysis to develop the electrocatalysts with many elemental steps, like OER and oxygen reduction reaction catalysts.
研究领域:
电化学
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催化
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材料科学
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产品关联
DOI
高影响因子
BIOELECTROCHEMISTRY
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2026
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IF 4.9
Zhenchao Li,Han Sun,Ying Zhang,Serge Cosnier,Aihua Liu
Biofuel cells (BFCs) are considered as green energy, which use enzyme biocatalysts to convert chemical energy into electrical energy, attracting great attention due to their potential applications in portable or implantable device. However, traditional enzymatic BFCs experienced low energy density and poor stability. Herein, we report on platinum nanoparticles (Pt NPs) assembling on filamentous phage to form rod-like Pt NPs@phage nanoarchitecture, which improved the stability of Pt NPs. The as-developed Pt NPs@phage exhibited direct electro-oxidation of glucose at lower potential of 0.081 V versus SCE under neutral pH condition. By simple chemical precipitation followed by oxidization, we also developed a nickel oxyhydroxide (NiOOH) nanoflowers (NFs) with excellent laccase-mimicking nanozyme activity, which exhibit superior electrocatalytic oxygen reduction reaction under neutral pH condition. Finally, a non-enzymatic glucose BFC was constructed using Pt NPs@phage as the anode catalyst and NiOOH NFs as the cathode catalyst. The as-assembled non-enzymatic glucose BFC registered output voltage of 534 mV and a maximum power density of 47.52 μW·cm −2 . This research is of great significance for exploring high-performance electrocatalysts and nanozymes as efficient cathode catalysts for developing non-enzymatic biofuel cells.
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DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2021
·Vol. 33
·期 11
·2005587
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IF 30.849
Ke Wang,Hongfang Du,Song He,Lei Liu,Kai Yang,Jinmeng Sun,Yuhang Liu,Zhuzhu Du,Linghai Xie,Wei Ai,Wei Huang
Layered γ-type iron oxyhydroxide (γ-FeOOH) is a promising material for various applications; however, its sheet-shaped structure often suffers from instability that results in aggregation and leads to inferior performance. Herein, a kinetically controlled hydrolysis strategy is proposed for the scalable synthesis of γ-FeOOH nanosheets arrays (NAs) with enhanced structural stability on diverse substrates at ambient conditions. The underlying mechanisms for the growth of γ-FeOOH NAs associated with their structural evolution are systematically elucidated by alkalinity-controlled synthesis and time-dependent experiments. As a proof-of-concept application, γ-FeOOH NAs are developed as electrocatalysts for the oxygen evolution reaction (OER), where the sample grown on nickel foam (NF) exhibits superior performance of high catalytic current density, small Tafel slope, and exceptional durability, which is among the top level of FeOOH-based electrocatalysts. Density functional theory calculations suggest that γ-NiOOH in situ generated from the electrooxidation of NF would induce charge accumulation on the Fe sites of γ-FeOOH NAs, leading to enhanced OER intermediates adsorption for water splitting. This work affords a new technique to rationally design and synthesize γ-FeOOH NAs for various applications.
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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产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2025
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IF 5.3
Yan Fang,Chengcheng Cai,Hiromi Yamashita,Xufang Qian,Yixin Zhao
Electrocatalytic CO 2 reduction reaction (CRR) to produce value-added chemicals offers a sustainable strategy to address energy crisis and climate change. However, the conventional CRR is always coupled with the anodic oxygen evolution reaction (OER), suffering from large overpotential, and high energy consumption. To overcome this, we proposed an alternative system by pairing CRR with the electrocatalytic oxidation of ethylene glycol (EGOR), a product derived from the depolymerization of polyethylene terephthalate (PET) plastic waste. This novel coupled system enabled the simultaneous production of formate on both electrodes, achieving the dual utilization of plastic waste and CO 2 . In this study, we developed a commercially viable system combining a robust NiOOH electrocatalyst synthesized through a facile electrodeposition for EGOR with a low-cost Bi 2 O 3 electrocatalyst for CRR. The NiOOH electrocatalyst achieved Faradaic efficiencies over 88 % for EG oxidation into formate within a broad potential window (1.4–1.8 V RHE ), while Bi 2 O 3 delivered Faradaic efficiencies more than 90 % for CO 2 -to-formate conversion within −0.8 to −1.2 V RHE . When integrated in a two-electrode configuration, the EGOR/CRR system produced formate at both electrodes with Faradaic efficiencies above 85 % across a wide cell voltage (2.0–2.6 V), requiring a ∼300 mV lower cell potential compared to the OER/CRR system. This coupled system reached commercial-level current densities above 200 mA cm −2 or 400 mA cm −2 at 3.0 V when implemented in the flow cell or the MEA cell, respectively. These results demonstrated the potential to use waste-derived reactants and commercially accessible eletrocatalytsts to realize energy-efficient and scalable conversion into formate.
研究领域:
电化学
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催化
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环境科学
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能量转换
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材料科学
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化学工程
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Shuo Wang,Yong Yan,Yongping Du,Yuguo Zhao,Tongxian Li,Dong Wang,Peter Schaaf,Xiayan Wang
Recently, Ni-based chalcogenides havedemonstrated remarkable activity and selectivity for alcohol electrooxidation, but the mechanisms remain debated. This study synthesizes Ni-based electrodeswith different chalcogen anion coordination on nickel nanorod arrays (NiO x /Ni,NiS x /Ni, and NiSe x /Ni NRAs). NiSe x /Ni NRAsshowcases superior performance (Faradaic efficiency 92.9%) in glycerolelectrooxidation reaction (GOR). In situ spectroscopy reveals that NiSecoordination inhibits deep oxidative reconstruction of the Ni-based interface, preventingNiOOH phase formation during GOR, enhancing activity and stability of NiSe x /NiNRAs. Conversely, NiS and NiO coordination lead to deep reconstruction with NiOOHphase formation, limiting GOR performance. Differently, during competingreaction of GOR, the oxygen evolution reaction (OER) leads to deepreconstruction of NiSex interface due to the instability of Ni-Sebonds, inducing performance degradation and dissolution of Se components. Furthermechanism investigation elucidates that the rate-determining step (RDS) ofGOR at the NiSe x interface involves oxidation of *C 2 H 3 O 3 intermediatesthrough H 2 O adsorption, favoring stable formate production.Contrarily, the RDS at the NiS x , NiO x , and NiOOHinterfaces predominantly focus on the decarboxylation of multi-carbon intermediates, raisingenergy barriers and over-oxidizing formate to CO 2 . These results providenew insights for designing Ni-based non-oxide catalysts forefficient and stable electrocatalytic oxidation.
研究领域:
电化学
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材料科学
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催化
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能源材料
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产品关联
DOI
高影响因子
Journal of the American Chemical Society
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2024
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IF 14.4
Weihang Li,Haoyang Jiang,Xiang Zhang,Bo Lei,Le Li,Haoshen Zhou,Miao Zhong
Electrified synthesis of high-value organonitrogen chemicals from low-cost carbon- and nitrogen-based feedstocks offers an economically and environmentally appealing alternative to traditional thermocatalytic methods. However, the intricate electrochemical reactions at electrode surfaces pose significant challenges in controlling selectivity and activity, especially for producing complex substances such as N,N-dimethylformamide (DMF). Herein, we tackle this challenge by developing relay catalysis for efficient DMF production using a composite WO2–NiOOH/Ni catalyst with two distinctive active sites. Specifically, WO2 selectively promotes dimethylamine (DMA) electrooxidation to produce strongly surface-bound (CH3)2N*, while nearby NiOOH facilitates methanol electrooxidation to yield more weakly bound *CHO. The disparity in binding energetics of the key C- and N-intermediates expedites C–N coupling at the WO2–NiOOH interface. In situ infrared spectroscopy with isotope-labeling experiments, quasi-in situ electron paramagnetic resonance trapping experiments, and electrochemical operating experiments revealed the C–N coupling mechanism and enhanced DMF-synthesis selectivity and activity. In situ X-ray absorption spectroscopy (XAS) and postreaction transmission electron microscopy (TEM) studies verified the stability of WO2–NiOOH/Ni during extended electrochemical operation. A Faradaic efficiency of ∼50% and a production rate of 438 μmol cm–2 h–1 were achieved at an industrially relevant current density of 100 mA cm–2 over an 80 h DMF production period. This study introduces a new paradigm for developing electrothermo relay catalysis for the sustainable and efficient synthesis of valuable organic chemicals with industrial potential.
研究领域:
电化学
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催化
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材料科学
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化学工程
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可持续化学
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Jiang Xiaoyi,Ke Le,Zhao Kai,Yan Xiaoyu,Wang Hongbo,Cao Xiaojuan,Liu Yuchen,Li Lingjiao,Sun Yifei,Wang Zhiping,Dang Dai,Yan Ning
Electrochemical carbon dioxide reduction reaction using sustainable energy is a promising approach of synthesizing chemicals and fuels, yet is highly energy intensive. The oxygen evolution reaction is particularly problematic, which is kinetically sluggish and causes anodic carbon loss. In this context, we couple CO 2 electrolysis with hydrogen oxidation reaction in a single electrochemical cell. A Ni(OH) 2 /NiOOH mediator is used to fully suppress the anodic carbon loss and hydrogen oxidation catalyst poisoning by migrated reaction products. This cell is highly flexible in producing either gaseous (CO) or soluble (formate) products with high selectivity (up to 95.3%) and stability (>100 h) at voltages below 0.9 V (50 mA cm −2 ). Importantly, thanks to the “transferred” oxygen evolution reaction to a water electrolyzer with thermodynamically and kinetically favored reaction conditions, the total polarization loss and energy consumption of our H 2 -integrated CO 2 reduction reaction, including those for hydrogen generation, are reduced up to 22% and 42%, respectively. This work demonstrates the opportunity of combining CO 2 electrolysis with the hydrogen economy, paving the way to the possible integration of various emerging energy conversion and storage approaches for improved energy/cost effectiveness.
研究领域:
电化学
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能源转换与存储
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可持续能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
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IF 8.3
Mingxin Cai,Qinghua Ye,Ziru Wang,Peilei He
Electrochemical water splitting for hydrogen production is currently constrained by the sluggish kinetics of the anodic oxygen evolution reaction (OER). NiFe-based catalysts have emerged as promising alternatives to precious metal OER catalysts due to their low cost and relatively high electrocatalytic activity. However, NiFe-based catalysts prepared by conventional synthesis methods suffer from a low density of exposed active sites and ambiguous structures. Herein, we report a straightforward solution-thermal strategy for constructing two-dimensional sub-1 nm nanosheets (SNSs) through the self-assembly of an iron-substituted polyoxometalate (FeMo 6 ) cluster with Ni 3 S 2 . The Ni 3 S 2 –FeMo 6 SNSs exhibit excellent electrocatalytic performance in 1 M KOH, achieving an overpotential of only 342 mV at a current density of 100 mA cm −2 and maintaining stability for 100 h at 10 mA cm −2 . The synergistic effect between Fe and Ni 3 S 2 effectively modulates the electronic structure of the catalyst, accelerating the formation of the active NiOOH phase. Furthermore, Fe incorporation actively enhances hydroxyl groups adsorption on the catalyst surface and facilitates lattice oxygen participation in the reaction. This work clarifies the role of Fe in NiFe-based electrocatalysts, providing new perspectives for developing facile-to-synthesize and high-performance electrocatalysts.
研究领域:
电化学
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纳米材料
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催化
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能量转换
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）