CATALYSIS LETTERS
·
2023
·Vol. 154
·期 5
·2182-2196
·
IF 2.8
Liu Jialu,Song Zhi,Liu Boxia,Zhang Xiayan,Huang Yeqiong,Han Dongxu
Because of its high toxicity and severe degradation, phenol has caused serious environmental pollution, and it is urgent to explore a stable and efficient degradation method of phenol. In this study, Ni/Fe bimetallic atomic cluster composite catalyst activated peroxymonosulfate (PMS) to degrade phenol efficiently. The experimental results show that the phenol degradation rate can reach 100% in a wide range of pH (3–11), and the system offers good stability in repeated experiments. The free radical quenching investigation and electrochemical characterization showed that the non-free radical pathway dominated the degradation system, and a large amount of singlet oxygen and rapid electron transfer promoted the efficient degradation of phenol in wastewater. This study opens up a new way for bimetallic atom cluster catalysts to activate PMS to degrade organic pollutants. Graphical
研究领域:
环境科学
·
催化
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
Carbon Energy
·
2024
·
IF 19.5
Zhi Cai,Mingyuan Xu,Yanhong Li,Xinyan Zhou,Kexin Yin,Lidong Li,Binbin Jia,Lin Guo,Hewei Zhao
The dynamic surface self-reconstruction behavior in local structure correlates with oxygen evolution reaction (OER) performance, which has become an effective strategy for constructing the catalytic active phase. However, it remains a challenge to understand the mechanisms of reconstruction and to accomplish it fast and deeply. Here, we reported a photo-promoted rapid reconstruction (PRR) process on Ag nanoparticle-loaded amorphous Ni-Fe hydroxide nanosheets on carbon cloth for enhanced OER. The photogenerated holes generated by Ag in conjunction with the anodic potential contributed to a thorough reconstruction of the amorphous substrate. The valence state of unsaturated coordinated Fe atoms, which serve as active sites, is significantly increased, while the corresponding crystalline substrate shows little change. The different structural evolutions of amorphous and crystalline substrates during reconstruction lead to diverse pathways of OER. This PRR utilizing loaded noble metal nanoparticles can accelerate the generation of active species in the substrate and increase the electrical conductivity, which provides a new inspiration to develop efficient catalysts via reconstruction strategies.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 37
·14306-14316
·
IF 4.569
Hao Wu,Qingxi Zhai,Fan Ding,Dongyue Sun,Yujie Ma,Yilun Ren,Biao Wang,Fengqi Li,Haifeng Bian,Yurong Yang,Lan Chen,Shaochun Tang,Xiangkang Meng
The preparation of low-cost and high-activity oxygen evolution reaction (OER) catalysts is a technical bottleneck in the field of electrolysis of water to produce hydrogen. Amorphous metal–organic frameworks (MOFs) with low-cost transition metals have attracted increasing attention in the catalytic field, yet metal atoms that are the main active sites are still ambiguous. Here, we synthesized a series of amorphous ternary Fex(NiCu)3−x-MOFs via an ultrasonic method. The optimal amorphous FeNiCu-MOF is found to be able to supply a current density of 10 mA cm−2 merely at a low overpotential of 260 mV with a small Tafel slope of 61 mV dec−1 and exhibits high durability over 24 h. Moreover, density functional theory (DFT) calculations show that the Fe atoms are the main active sites for the OER in the FeNiCu-MOF. This work shows that amorphous ternary MOFs have great potential for application in OER electrocatalysts due to the multiple synergistic effects and amorphous MOF structures.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Xiaodong Chen,Ning Wang,Kui Shen,Yangkai Xie,Yongpeng Tan,Yingwei Li
In order to improve the catalytic performance of oxygen reduction reaction (ORR), it is pivotal to increase the density and accessibility of the active sites. Herein, we have developed a template-free melamine-assisted cocalcined strategy to afford Fe-embedded and N-doped carbons (Fe–N–C) with not only high density of atomically dispersed Fe–Nx active sites but also abundant three-dimensional interconnected mesopores by directly pyrolyzing Fe-ZIF-8 covered with a controllable melamine layer. It is demonstrated that the introduction of melamine in the precursor plays a key role in constructing various carbonized products with controllable morphology, porosity, and components. With an optimal mass ratio 1:1 of melamine to Fe-ZIF-8, the resultant Fe@MNC-1 exhibits excellent ORR activity and stability, which exceeds 20 wt % commercial Pt/C catalyst (with a half-wave potential of 0.88 V vs 0.85 V) in an alkaline electrolyte and is even comparable to the commercial Pt/C catalyst (with a half-wave potential of 0.78 V vs 0.80 V) in an acidic electrolyte. To the best of our knowledge, Fe@MNC-1 can be ranked among the best nonprecious metal electrocatalysts for ORR in both alkaline and acidic media. The present synthetic strategy may provide a new opportunity for the design and construction of metal–organic framework-derived nanomaterials with rational composition and a desired porous structure to boost their electrocatalytic performance.
研究领域:
材料科学
·
电化学
·
催化
·
纳米材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2025
·
IF 12.1
Hui-Min Xu,Kai-Hang Yue,Hong-Cheng Zhang,Xiao-Qi Gong,Shao-Lan Zheng,Meng-Han Yin,Guang-Hui Xia,Gao-Ren Li
In recent years, zinc-air battery (ZAB) has received great attention because of their high energy density, low manufacturing cost, environmental friendliness, and high safety. The main obstacle to the widespread use of ZAB is the design and preparation of low-priced and high-performance electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Herein, the paired Fe single-atoms with Se, N-atom coordination supported on N, S-codoped carbon (FeN x Se y @SNC) are designed and synthesized as catalyst for ZABs. The physical and chemical characterizations indicate the existence of paired Fe single-atoms. The FeN x Se y @SNC exhibits exceptional ORR catalytic activity with a half-wave potential ( E 1/2 ) of up to 0.92 V RHE and an onset potential ( E onset ) of 1.057 V RHE and a overpotential of 346 mV for OER at 10 mA cm −2 . The FeN x Se y @SNC-based ZAB shows a high peak power density of 307 mW cm −2 at 475 mA cm −2 , a high specific energy density of 760.9 mAh g −1 at 10 mA cm −2 , and superior long-term durability. DFT reveal that the asymmetric Fe─Se─Fe bridging bonds and S-atom coordination in the Fe 2 N 5 SeS allow precise control of Fe active sites, and can well modulate the electronic properties of Fe sites, optimize the adsorption energies of oxygen intermediates and improve catalytic performance.
研究领域:
电化学
·
能源材料
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催化
·
材料科学
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可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Physics
·
2021
·
IF 9.298
A. Wang,Y. Hu,H. Wang,Y. Cheng,T. Thomas,R. Ma,J. Wang
To improve the structure-dominant activity, rational design of oxide-based materials remains challengeable in bifunctional oxygen electrocatalysis , especially from the perspective of electronic modulation. Herein, we demonstrate that the electron configuration of inverse spinel NiCo 2 O 4 can be activated by controllable substitution of Fe into the octahedral centers. Fe-substituted NiCo 2 O 4 nanoparticles embedded in porous N-doped carbon nanofibers (NiCo 2- x Fe x O 4 /NCNF), which were synthesized by scalable electrospinning, exhibit a correlated relationship with Fe atomic content and achieve an optimal bifunctional activity (ΔE = 0.74 V) at 0.25 at.%. Theoretical calculation shows that the substitution of Co 3+ by Fe 3+ modulates the electrons filling in e g orbital of octahedral cation via delocalizing the electrons around O anions. The increased density of states around the Fermi level further regulate the adsorption energy of oxygen intermediates and lead to better bifunctional performance than commercial Pt/C + RuO 2 in rechargeable Zn-air battery. This work provides a new pathway to develop cost-effective bifunctional electrocatalysts for electrochemical energy storage and conversion .
研究领域:
材料科学
·
电化学
·
储能与转换
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）