APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Liming Dai,Chenchen Fang,Fanglei Yao,Xiaoyuan Zhang,Xuefeng Xu,Shangling Han,Jingyao Deng,Junwu Zhu,Jingwen Sun
In-situ generated hydroxides and oxyhydroxides have been gradually recognized as the real active sites of metal organic frameworks (MOFs) towards the oxygen evolution reaction (OER). Nevertheless, the fine phase evolution process is still less of concern and elusive. Herein, we successfully construct serious of Ni-MOFs with differing thickness ranging from 1 nm to 270 nm through a competitive coordination strategy. Utilizing the operando resonance spectroscopy, an accurate phase inversion behavior of the Ni-MOFs has been witnessed during the OER, and demonstrated as a thickness-dependent process. Ultrathin architecture is identified as a positive factor to promote the exchange between MOFs ligands and applied electrolyte during the electrochemical test. Hence, after removing most of the internal ligands, 2D MOFs favor to be transformed as β-NiOOH, which is more active than the generated γ-NiOOH in bulky system. The density function theory (DFT) calculation alongside with the in-situ electrochemistry tests further affirm the β/γ-NiOOH transformation behavior. This work offers a new understanding of the electrocatalytic mechanism from the view point of phase evolution in 2D MOFs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Yifei Huang,Xuliang Pang,Jianguo Cui,Zhenzhen Huang,Guanhua Wang,Huaiquan Zhao,Hongye Bai,Weiqiang Fan
Electrochemical oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) is a promising approach to produce high-value chemicals such as 2,5-furandicarboxylic acid (FDCA). However, the undesirable stability of catalysts commonly limits its potential application value. In this work, NiOOH derived from Ni(OH)2 was determined as the main catalytic site for HMF oxidation, but the collapse of Ni(OH)2 caused severe instability during the electrocatalytic process because of the crystal structure mismatch between NiOOH and Ni(OH)2. The implantation of Ce in Ni(OH)2 (Ce-Ni(OH)2) was successfully realized to address the stability issue of bare Ni(OH)2, since the larger ion radius of Ce could increase the Ni–O bond length and d-spacing. As a result, the activity of 14%Ce-Ni(OH)2 has not obviously decayed after the 50 cyclic voltammetry (CV)-cycle test. HMF conversion is close to 100%, and the Faraday efficiency (FE) reaches 86.6% at the potential of 0.45 V vs Ag/AgCl. This study provides a new strategy to design stable catalysts for the conversion of biomass derivatives.
研究领域:
电化学
·
催化材料
·
生物质转化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2015
·
IF 4.504
Mingshu Xiao,Yanping Tian,Yuhua Yan,Kai Feng,Yuqing Miao
In order to lower the energy barrier and improve the energy efficiency for hydrogen production by splitting water, highly efficient OER catalysts are required. Here, we report the electrodeposition of Ni(OH) 2 /NiOOH in the presence of urea showing the improved electrocatalysis for the hydrogen production in KOH electrolyte. By potential scanning, the Ni(OH) 2 colloid in alkali solution was transformed into the deposited Ni(OH) 2 /NiOOH. The presence of urea facilitates to deposit Ni(OH) 2 /NiOOH with higher electron transfer than the absence of urea, leading to a higher electrocatalytic OER. As supporting electrolyte , KOH exhibits better performance on the electrodeposition of Ni(OH) 2 /NiOOH and their OER electrocatalysis than NaOH. The work shows the potential application using cheap, non-precious metal-based electrocatalysts to overcome the well-known bottlenecks limiting power density of hydrogen fuel cell and energy efficiency of splitting water.
研究领域:
电化学
·
催化材料
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Liuqing Wang,Jinsheng Li,Qinglei Meng,Meiling Xiao,Changpeng Liu,Wei Xing,Jianbing Zhu
The insufficient performance of non-noble metal catalysts in alkaline media is a prominent issue that limits the widespread adoption of electrocatalytic water splitting. In this study, we present an efficient Mo doping strategy to boost the electrocatalytic performance of NiFe layered double hydroxide (LDH) through modulating the electronic structure of active Ni sites. The optimized Mo doped NiFe-LDH (denoted as NiFeMo-2) exhibits significantly improved activity, showing a smaller overpotential of 262 mV at 10 mA cm−2 compared to NiFe-LDH (344 mV). X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) spectra demonstrate that the incorporation of Mo not only increases the electron cloud density of Ni, but also induces more oxygen vacancies. Due to these structural modifications, the oxygen evolution reaction (OER) kinetics is dramatically enhanced, confirmed by in situ electrochemical impedance spectroscopy (EIS). Moreover, in situ Raman spectroscopy shows that the Mo doping can facilitate the formation of active NiOOH species at a lower potential, thus accelerating the OER kinetics. The in situ differential electrochemical mass spectrometry (DEMS) technique with 18O isotope labelling, tetraalkylammonium cation (TMA+) chemical probe, and ethanol oxidation reaction suggest that the NiFeMo-LDH catalyst primarily follows the adsorbate evolution mechanism (AEM) pathway, the promoted dehydrogenation process with the modulation of *OH adsorption. This study reports a high-performance non-noble metal OER electrocatalyst and unveils the origins of metal doping to enhance the OER kinetics.
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2020
·
IF 5.278
Minxuan Li,Xu Xu,Lei Zhang
In this paper, oleophilic and superhydrophobic sponges were successfully constructed via a one-pot low temperature hydrothermal method anchoring three-dimensional rambutan-like-β-NiOOH microspheres into sponge skeletons and lauric acid modification. The constructed modified three-dimensional rambutan-like-β-NiOOH @sponge (the static contact angle of 153.5°) possessed outstanding oil sorption capacity (separation efficiency is nearly 99%) towards the various organics/oils and excellent recyclability after 30 cycles of adsorption-squeezing. Importantly, modified three-dimensional rambutan-like-β-NiOOH @sponge is capable of separating surfactant-stabilized water-in-oil emulsions and can be utilized for continuous oil-water separation with the aid of a peristaltic pump. This is mainly due to the fact that the three-dimensional hierarchical rambutan-like micronano structure formed by self-assembly with high specific surface area provides a large number of hydrophobic interfaces to improve the hydrophobic properties of sponges. This work presents a new strategy for the designs multitasking oil-water separation materials.
研究领域:
材料科学
·
环境工程
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Jing Chen,Sijie Chen,Jinghao Gao,Xiaowu Huang,Elissaios Stavrou,Charlotte Vogt,Weiran Zheng
The electrochemical ammonia oxidation reaction (AOR) offers a promising pathway for environmental remediation, energy conversion, and the production of value-added chemicals. Although NiOOH shows potential as an efficient catalyst for AOR, the underlying mechanism and the influence of the concurrent oxygen evolution reaction (OER) are not yet fully understood. Here, the AOR mechanism on NiOOH is examined, emphasizing the influence of OER and dissolved O 2 . Using differential electrochemical mass spectrometry (DEMS), Raman spectroelectrochemistry, UV–vis spectroelectrochemistry, and attenuated total reflection infrared reflection (ATR-IR) spectroelectrochemistry, we reveal that the NiOOH formation, AOR activity, selectivity, and deactivation as well as the reaction intermediates are significantly modulated by OER and dissolved O 2 . AOR on NiOOH is potential-dependent: N 2 production starts with the onset of OER, while extensive NO x and NO 2/3 − species form at higher potentials. The OER competes with the AOR-to-N 2 pathway but promotes AOR-to-NO x , where the presence of O 2 mitigates OER deactivation on NiOOH. Our findings highlight the advantage of correlative in situ analysis in studying electrocatalytic processes and advance the current understanding of AOR pathways on NiOOH toward energy and environmental applications.
研究领域:
环境科学
·
能源科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Guozhen Fang,Xiaowen Ruan,Depeng Meng,Minghua Xu,Chunsheng Ding,Chengxiang Huang,Yu Qiu,Shengli Zhao,Kaikai Ba,Tengfeng Xie,Yong Zhou,Haiyan Zhang,Wei Zhang,Shengye Jin,Jing Leng,Sai Kishore Ravi,Xiaoqiang Cui
The four-electron water oxidation reaction in photoelectrochemical systems poses a major challenge to efficiently converting solar energy into chemical energy amid the global energy crisis. Herein, we report a strategy to develop a photoelectrochemical system using BiVO 4 /Bi 4 V 2 O 10 isometallic heterojunction photoanodes paired with FeOOH/NiOOH cocatalysts to enhance water oxidation in neutral electrolytes. The results demonstrate that the BiVO 4 /Bi 4 V 2 O 10 /FeOOH/NiOOH photoanode achieves a photocurrent density of 4.48 mA/cm 2 at 1.23 V versus the reversible hydrogen electrode and an applied bias photon-to-current efficiency of 1.69 % at 0.63 V versus the reversible hydrogen electrode—significantly outperforming bare BiVO 4 . This enhanced photoelectrochemical performance is attributed to the identical elemental composition and well-aligned energy band positions of Bi 4 V 2 O 10 and BiVO 4 , which minimize charge recombination at the interface. Additionally, the FeOOH/NiOOH double-layer cocatalyst facilitates rapid transfer of photogenerated carriers, as confirmed by femtosecond transient absorption spectroscopy and transient photovoltage measurements. This approach provides a novel and effective pathway for advancing high-efficiency photoelectrochemical cells.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysts
·
2024
·Vol. 14
·期 8
·496
·
IF 3.8
Kaige Zhao,Xinhao Xu,Manli Wang,Tao Chen,Qianlin Ju,Lulu Hao,Zelin Chen,Xiaolong Yu,Changjiu Li
The electrocatalytic oxidation of urea combined with wastewater splitting is considered a promising approach for sustainable hydrogen production, characterized by minimal energy consumption. However, its evolution is greatly hindered by the shortage of efficient and easily accessible electrocatalytic materials. Here, a facile electrochemical activation strategy was conceived and proposed to construct a Cu-doped NiOOH nanolayer encapsulated on Cu2O nanodendrites on Cu mesh substrate (Cu-NiOOH/Cu2O/CM) from the electrodeposited Ni/Cu2O/CM heterostructured precatalyst. It was verified that the incorporation of Cu not only facilitates the rapid formation of Ni(III)species but also contributes to the formation of Cu-Ni(III)bifunctional electrocatalytic active sites. Benefiting from the accessible Cu-Ni(III)dual active sites, high active surface area, good hydrophilic and aerophobic surface properties and superior electrical conductivity of the Cu mesh substrate, the as-prepared Cu-NiOOH/Cu2O/CM exhibits enhanced bifunctional electrocatalytic abilities for electrocatalytic urea oxidation reaction (UOR) and hydrogen evolution reaction (HER). Particularly, for the Cu-NiOOH/Cu2O/CM||Cu-NiOOH/Cu2O/CM configuration toward the UOR||HER coupled system, a significantly reduced cell voltage of 1.43 V vs. RHE @ 10 mA·cm−2was obtained. The observed cell voltage for the conventional overall water splitting is approximately 190 mV higher than that observed for overall urea splitting. This study proposes a viable approach to achieve and optimize the bifunctional UOR/HER performance of NiOOH active species, which holds significant importance for efficient and stable hydrogen generation from urea-contaminated substandard water.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jianlong Zhang,Jinlv Wei,Zhixiang Zhai,Huan Wen,Boyao Feng,Xizi Wu,Dexin Meng,Jia Wu,Shibin Yin
NiOOH generated in situ from pre-catalysts plays a key role in the 5-hydroxymethylfurfural electrooxidation reaction. However, the dynamic structural evolution of NiOOH remains relatively difficult and unclear. In this work, we focus on V-Ni 3 N as a case study. Density functional theory calculations, in-situ spectroscopy, and experimental results demonstrate that the V doping modulates the charge redistribution between the nickel and nitrogen in Ni 3 N and weakens the covalency of the Ni−N bonds, leading to easier formation of N vacancies and enhanced adsorption of OH* on Ni 3 N catalyst. This facilitates the transformation of the Ni−N bond into the Ni−O bond, thereby promoting the formation of active NiOOH for HMF oxidation. In addition, the doped V atoms enhance the interaction between NiOOH and HMF molecules and reduce the energy barrier of the rate-determining step. Thus, V-Ni 3 N/CC presents an excellent catalytic performance in terms of high 2,5-furandicarboxylic acid selectivity.
研究领域:
化学
·
材料科学
·
电催化
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 43
·2106904
·
IF 15.153
Zhong Wu,Yanhui Feng,Zhenbo Qin,Xiaopeng Han,Xuerong Zheng,Yida Deng,Wenbin Hu
Development of efficient non-noble metal catalysts for water splitting is of great significance but challenging due to the sluggish kinetics of the hydrogen evolution reaction (HER) in alkaline medium. Herein, a bimetallic multi-level layered catalytic electrode composed of Ni 3 S 2 nanosheets with secondary Co-NiOOH layer of 3D porous and free-standing cathode in alkaline medium is reported. This integrated synergistic catalytic electrode exhibits excellent HER electrocatalytic performance. The resultant Ni 0.67 Co 0.33 /Ni 3 S 2 @NF electrode displays the highest HER activity with only overpotentials of 87 and 203 mV to afford current densities of 10 and 100 mA·cm −2 , respectively, and its Tafel slope is 80 mV·dec −1 . The chronopotentiometry operated at high current density of 50 mA·cm −2 shows negligible deterioration, indicating better stability of Ni 0.67 Co 0.33 /Ni 3 S 2 @NF electrode than Pt/C (20 wt.%). Such a desirable catalytic performance is attributed to the modification of physical and electronic structure that exposes abundant active sites and improves the intrinsic catalytic activity toward HER, which is also confirmed by electrochemically active surface area and X-ray photoelectron spectroscopy analysis. This work provides a strong support for the rational design of high-performance bimetallic electrodes for industrial water splitting.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2020
·
IF 0
Qingnan Wu,Ming Wen,Weixi Yan,Qingsheng Wu,Hezhong Wang,Yongqing Fu
A functionalized carbon nanotube (FCNT)/Ni(HCO3)2-Ni nanostructures were synthesized by decorating nanoflaky and mesoporous Ni(HCO3)2 onto FCNT along with in situ formed reduced metallic Ni for the purpose of constructing an energy-storage system with both high specific capacity and cycling stability. Such flaky nanostructures can significantly increase the contact surface areas between the mesoporous and nanoflaky Ni(HCO3)2-Ni and electrolyte, thus immensely reducing the electrolyte-ion diffusion paths and accelerating the electron-transport rates through the use of a FCNT. The in situ reduced metallic Ni atoms are directly contacted with the electrolytes and quickly converted into NiOOH in the alkaline environment. For this reason, the capacity retention of battery-type electrochemical materials can be significantly enhanced, especially at the beginning of cycles. The obtained flaky FCNT/Ni(HCO3)2-Ni nanomaterials exhibit excellent electrochemical performances with a high specific capacity of 203 mAh·g–1 at 3 A·g–1 current density for supercapacitor energy-storage systems. An aqueous asymmetric supercapacitor made of FCNT/Ni(HCO3)2-Ni//graphene oxide achieves a 132 Wh·kg–1 energy density at 2880 W·kg–1 power density and an excellent cycling stability with 84% after 6000 cycles.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
·
2023
·
IF 2.7
Zhongying Fang,Xiaolong Liang,Lehui Lu,Wei Chen
The electrocatalytic oxidation of urea (EOU) is an important half-reaction in water splitting, urea fuel cells, and urea wastewater treatment. The anions of nickel-based catalysts can be leached severely in the oxidation potential range. Therefore, the influence of anion on the electrocatalytic performance of Ni(OH) 2 /NiOOH for urea oxidation has not been systematically studied. The present experimental results show that the structure reconstruction of catalyst is a complicated process, specifically including deep penetration by alkaline electrolyte, leaching-induced oxidation by phosphorus or sulfur anions, transformation or cracking of the original structure, and formation of an amorphous layer on the surface. The reconstructed NF-NiP x -R or NF-NiS x -R has a three-layer core-shell structure, with a nickel foam skeleton in the innermost layer, an amorphous NiP x or NiS x layer in the middle layer, the outermost layer of oxygen-containing anion (PO x or SO x ) coordinated Ni(OH) 2 . In the prepared catalyst, the Ni(OH) 2 /NiOOH redox is the real catalytic species for the urea oxidation. It is found that the oxygen-containing anion can enhance the catalytic performance of the Ni(OH) 2 /NiOOH redox, and PO x anion has the best enhancing effect. It is found that the urea molecules are oxidized on the electrocatalyst surface mainly through an indirect pathway.
研究领域:
电化学
·
催化材料
·
环境科学
✓ 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）