Science Bulletin
·
2018
·
IF 4.136
Qingfeng Xu,Wenlong Chen,Yucong Yan,Zhemin Wu,Yi Jiang,Junjie Li,Ting Bian,Hui Zhang,Jianbo Wu,Deren Yang
Incorporating Pt with core metals into Pt-based core-shell catalysts is regarded as a promising strategy to substantially enhance the catalytic properties towards oxygen reduction reaction (ORR) in fuel cells due to the synergetic effect between distinct metals. In this wok, ultrathin Pt skins with two atomic layers were epitaxially coated on as-prepared icosahedral Au 50 Pd 50 , Au 60 Pd 40 and Au 66 Pd 34 nanocrystal seeds, which are constructed with alloyed cores and Pd shells with different thickness. Through electron microscopic characterizations, Pd interlayers with tunable thickness of 3, 6, and 12 atomic layers can be found in the Au 66 Pd 34 @Pt, Au 60 Pd 40 @Pt and Au 50 Pd 50 @Pt icosahedra, respectively. These icosahedral AuPd@Pd@Pt nanocrystals show substantially enhanced activities and durabilities in electrocatalytic measurements towards ORR compared to Au 75 Pd 25 @Pt icosahedra without Pd interlayer and commercial Pt/C catalysts. Specifically, Au 60 Pd 40 @Pt icosahedra with 6 atomically thick Pd interlayer display the best electrocatalytic performances, whose mass activities before and after durability tests of 50,000 cycles are 11.6 and 30.2 times, respectively, as high as that of the commercial Pt/C.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 3
·273
·
IF 4.501
Zicong Zhang,Xiangli Ru,Xiaoli Yang,Zhengyu Bai,Lin Yang
In addition to C, H and O, some biomass is also rich in mineral elements. The recovery and utilization of special mineral elements is of great significance to prepare functional materials and alleviate the current energy shortage. Herein, we describe a facile strategy for making full use of the chemical composition (C, Fe) and special structure of red blood cells (RBCs) from waste pig blood to fabricate a dual metal (Fe, Co)-nitrogen (N)-doped porous carbon catalyst by pyrolysis of a mixture of RBCs biomass, cobaltous acetate, and melamine. The porous catalyst displays a comparable activity for oxygen reduction reaction (ORR) to that of commercial Pt/C catalyst, with a half-wave potential of 0.821 VvsRHEin alkaline media and 0.672 VvsRHEin acid electrolyte. Especially, the as-prepared catalyst shows excellent methanol tolerance and stability in both acidic and alkaline electrolytes, which is superior to commercial Pt/C catalysts. The excellent ORR activity of FeCo-N/C(RBC)can be ascribed to the porous morphology and the cooperation between metal and nitrogen species. This work provides a novel idea of exploiting the composition of renewable biomass to modulate the activity and stability of carbon-based ORR catalysts.
研究领域:
材料科学
·
生物医学工程
✓ 已验证
DOI
高影响因子
TRANSITION METAL CHEMISTRY
·
2025
·
IF 1.7
Wang Yuqin,He Lizi,Han Ning,Li Lishuang,Wang Meiyang
It is of great practical significance to explore and prepare cheap, high-performance, and stable catalysts for oxygen reduction reaction (ORR), but it is still in progress at present. Herein, a straightforward evaporation–pyrolysis strategy is designed for the preparation of 3D porous electrocatalysts (denoted as \(\textrm{Fe}-\textrm{Co}-\textrm{NC}\) , which represented carbonization products at °C) made of carbon nanoparticles combined with metallic Fe-Co-doped N-enriched bridged carbon nanotube by carbonization of a pristine ZIF8 as highly efficient and durable ORR electrocatalysts. The obtained Fe–Co–NC structure possesses 3D open porous texture, abundant active sites, desired nitrogen bonding type, and high specific surface area, providing them with excellent ORR activity. The optimal performing \(\textrm{Fe}-\textrm{Co}-\textrm{NC}\) catalyst presents an outstanding ORR performance in terms of a high onset potential ( \(\textrm{E}_{\text{ onset } }\) ) of 0.96 V (vs. RHE) and half-wave potential ( \(\textrm{E}_{1 / 2}\) ) of 0.86 V (vs. RHE), respectively, possible to rival those of the commercially available \(\textrm{Pt} / \textrm{C}\) in an alkaline electrolyte solution. Besides, the \(\textrm{Fe}-\textrm{Co}-\textrm{NC}\) catalyst manifests better stability than those of commercially available \(\textrm{Pt} / \textrm{C}\) , which is of importance for the optimization and characterization of novel electrocatalysts originated from non-precious metals.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Lilian Wang,Li Yang,Xinyu Zhao,Hang Ma,Bohuai Pang,Lingyan Duan,Kun Zeng,Lu Liu,Anran Chen,Hong Guo
The strong perturbation of the valence band within the entire material system and accelerated *OH dissociation from Fe site are triggered by incorporating CrN 4 moiety with low Fenton effect and *OH adsorption energy. This atomically dispersed Cr=N 2 =Fe electrocatalyst is developed by adopting a super time-/energy-saving Joule heating strategy (∼ 10 s). Through the investigation of valence orbital energy levels and valence electron behavior for the prepared catalysts, in combination with in-situ Raman testing and theoretical calculations, we have determined that the interaction between the metal sites and oxygen-containing intermediates primarily depends on orbital energy levels before being further evaluated by bond order involving electronic modulation. This finding may offer a valuable insight for future research in related electrocatalysis fields. The Cr=N 2 =Fe catalyst exhibits higher ORR catalytic capability than commercial Pt/C, thus driving stable operation of the assembled zinc-air battery for over 300 h.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jiahao Liu,Zhaorui Zhang,Chenshuai. Han,Zhihang Xu,Ye Zhu,J. Paul Attfield,Jianrong Zeng,Minghui Yang
Hydrogen peroxide (H 2 O 2 ) is a clean and versatile oxidant with significant applications in marine pollution treatment. Direct electrosynthesis of H 2 O 2 via the two-electron oxygen reduction reaction (2e - ORR) from seawater offers a sustainable and efficient alternative by eliminating the need for H 2 O 2 transport and storage. Herein, we report a 2-bromothiophene-modified nickel nitride (D-Ni 3 N) catalyst that optimizes oxygen adsorption to selectively enhance the 2e - ORR pathway while mitigating halide-induced corrosion and alkaline earth salt precipitation. D-Ni 3 N achieves a remarkable H 2 O 2 yield rate of 4.69 mol·h −1 ·g −1 with a Faradaic efficiency of 94.6 %, sustaining continuous operation for over 120 hours in natural seawater. Notably, the capital cost of 70 wt% H 2 O 2 is remarkably low at just $0.20 kg −1 . This work highlights the transformative potential of ligand-modified metal nitrides as stable and efficient 2e - ORR catalysts for sustainable H 2 O 2 production in seawater purification applications.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2014
·Vol. 19
·期 2
·497-506
·
IF 2.234
Jiang Liqing,Cui Lili,He Xingquan
Cobalt 5,10,15,20-tetrakis(4-pyridyl)porphyrin (CoTPyP) micro/nanoparticles assembled on poly(sodium-p-styrenesulfonate) (PSS) modified reduced graphene oxide (PSS-rGO) as a nonnoble catalyst for oxygen reduction reaction (ORR) was prepared by an in situ solvothermal synthesis method. The CoTPyP/PSS-rGO micro/nanocomposite was characterized by UV-vis spectroscopy, X-ray photoelectron spectroscopy (XPS), and scanning electron microscope (SEM) techniques. Cyclic voltammetry (CV) measurement result disclosed that CoTPyP/PSS-rGO possesses quite high electrochemically accessible surface area, which was more than tripled as large as the bare glassy carbon (GC) electrode. Rotating disk electrode (RDE) and rotating ring-disk electrode (RRDE) techniques were employed to study the catalytic activity and the ORR mechanism of as-synthesized CoTPyP/PSS-rGO catalyst in an alkaline medium. Linear sweep voltammetry (LSV) tests showed that the half-wave potential for ORR on the CoTPyP/PSS-rGO catalyst was found to be around −0.22 V vs. saturated calomel electrode (SCE), which was similar to that on Pt/C (−0.20 V vs. SCE). RRDE results displayed that the percentage of hydrogen peroxide yielded on the CoTPyP/PSS-rGO composite was less than 20 %, and the ORR process mainly proceeded via an almost direct 4-electron pathway. Moreover, the assembled CoTPyP/PSS-rGO catalyst possessed good stability and excellent tolerance to the crossover effect of methanol for ORR.
研究领域:
电化学
·
纳米材料
·
能源材料
·
催化化学
·
表面科学
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Fang Liu,Yang Liu,Dazhi Gao,Shaokai Ma,Shiqing Zhang,Ying Li,Jun Zhang,Yanming Xue,Chengchun Tang
Studying noble-metal-free oxygen reduction reaction (ORR) catalysts is crucial for advancing fuel cells. Manganese dioxide (MnO 2 ) has garnered widespread attention due to its convenient synthesis, low cost, high electrochemical activity, and diverse structures. However, it still faces challenges, such as poor conductivity and relatively lower inherent catalytic activity. In this study, a novel ORR electrocatalyst is introduced by constructing a heterostructure of manganese fluoride (MnF 2 ) and MnO 2 , referred to as MnF 2 /MnO 2 . In a 0.1 M KOH solution, the ORR half-wave potential (E 1/2 ) of MnF 2 /MnO 2 is measured at 0.804 V, surpassing that of the original MnO 2 catalyst (0.69 V). Compared to the MnO 2 electrocatalyst, the MnF 2 /MnO 2 heterostructure exhibits faster ORR reaction kinetics and a larger electrochemically active surface area. Density functional theory (DFT) calculations confirm that the MnF 2 /MnO 2 heterostructure possesses enhanced intrinsic conductivity, facilitating the rapid transfer of ions of and electrons. Therefore, this study provides a promising pathway for enhancing the ORR catalytic activity of noble-metal-free electrocatalysts through rational heterostructure design.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
MATERIALS TECHNOLOGY
·
2021
·
IF 3.846
Juanjuan Yin,Yuanyuan Guo,Zhiwei Liu,Qingrui Zhang,Tifeng Jiao
The energy problem is closely related to the survival and development of human beings. Nowadays, the research of fuel cells is making rapid progress, but the bottleneck of the development of fuel cells is slow oxygen reduction reaction (ORR) of cathode. At present, it is difficult to develop a kind of oxygen reduction catalyst with high performance, low energy consumption and low pollution. Here, we synthesised Co3O4 nanocrystals loaded on a single graphene oxide layer via a convenient one-step hydrothermal method. According to the transmission electron microscopy characterisation tests, the average size of Co3O4 nanocrystals is 5 nm. Compared with the commercially available Pt/C catalyst, the obtained Co3O4/rGO catalyst demonstrates the same four-electron (4e−) oxygen reduction reaction, and the catalytic activity of ORR is significantly higher. This is due to the large surface area provided by the middle part of the composite catalyst Co3O4/rGO, which provides an effective mass transfer and electron transfer path for the catalyst.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 9
·090512
·
IF 4.316
Yuebing Wang,Dunpeng Yang,Aling Chen,Qingfeng Yi
The development of an efficient, stable and low-cost cathode catalyst is necessary for the practical application of Zn-air batteries. In this paper, Fe3+/Co2+ ions were in situ incorporated into polydopamine during the polymerization of dopamine on the surface of the SiO2 spheres. After subsequent pyrolysis and leaching SiO2, the products loaded with different metals (NHCS-Fe, NHCS-Co, NHCS-Fe1Co0.6, NHCS-Fe1Co4, NHCS-Fe1Co10) were obtained. The samples possess a typical hollow carbon sphere (HCS) structure and show efficient oxygen reduction reaction (ORR) performance under neutral and alkaline conditions. Especially in the neutral electrolyte, the NHCS-Fe exhibits the comparable electrochemical catalytic activity to the commercial Pt/C. For NHCS-Fe, its ORR half-wave potential in neutral and alkaline media is 0.78 V and 0.83 V respectively. Corresponding neutral Zn-air battery reveals a maximum power density of 118.8 mW·cm−2, while they are respective 0.82 V and 46.99 mW·cm−2 for Pt/C. Alkaline Zn-air battery with NHCS-Fe releases a maximum power density of 262.4 mW·cm−2, displaying superior performance to Pt/C. Our work is instructive for the synthesis of novel ORR catalysts with outstanding activity by a versatile synthesis strategy.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 6
·期 5
·2264-2272
·
IF 8.867
Jing Li,Hu Zhou,Han Zhuo,Zhongzhe Wei,Guilin Zhuang,Xing Zhong,Shengwei Deng,Xiaonian Li,Jianguo Wang
The key bottleneck of applying Pd catalysts in fuel cells is their low activity and poor stability during the oxygen reduction reaction (ORR) although less precious Pd is still a promising alternative to Pt. Hence, new strategies to improve the performance of Pd in the ORR need to be developed. In this study, supported Pd (3.6 nm in average) catalysts on TiO2 with and without oxygen vacancies (VO) have been prepared via facile pyrolysis. Compared with commercial Pt/C (20 wt%) and Pd/TiO2 catalysts, Pd/TiO2-VO (10 wt%) demonstrated superior oxygen reduction activity, better durability, and higher methanol tolerance capability in alkaline solution. By means of experimental characterizations (ESR and XPS) and density functional theory (DFT) calculations, electron transfer from TiO2-VO to Pd nanoparticles (NPs) led to an electron-rich Pd surface and strong metal–support interactions (SMSIs). The electron-rich Pd NPs enhanced the adsorptions of key intermediates, lowered the Gibbs free energy of the ORR, and improved the ORR activity. SMSIs between Pd NPs and TiO2-VO endowed the catalyst with excellent stability and immunity to methanol poisoning. Therefore, the electron transfer from TiO2-VO to Pd NPs plays a crucial role in promoting the ORR performance of Pd-based electrocatalysts, which may be a new strategy to design high-performance ORR catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 10
·5382-5387
·
IF 2.936
Yong Qin,Fan Li,Peng Tu,Yanling Ma,Wenlong Chen,Fenglei Shi,Qian Xiang,Hao Shan,Lifu Zhang,Peng Tao,Chengyi Song,Wen Shang,Tao Deng,Hong Zhu,Jianbo Wu
We have demonstrated Ag3PO4 as an active non-Pt electrocatalyst with enhanced activity compared with Ag for oxygen reduction reaction (ORR). Density functional theory reveals that better ORR performance of Ag atoms on Ag3PO4 surface than that on pure silver surface originates from more appropriate oxygen adsorption on positively charged Ag atoms. Further study of the surface geometry of Ag3PO4 including tetrahedron, rhombic dodecahedron and cube indicates that the highest density of Ag and appropriate oxygen adsorption on {110} surface of rhombic dodecahedral Ag3PO4 lead to the highest ORR activity, which is about 12 times that of Pt catalysts from a commercial perspective. It may be applicable for developing low-cost and highly active non-Pt catalytic materials from a broader range of material systems.
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
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 14
·6065-6073
·
IF 9.931
Haoxiong Nan,Dai Dang,Xin Long Tian
The development of both effective and robust catalysts is crucial for the commercialization of polymer electrolyte membrane fuel cells since the reactivity and durability of the catalysts determine its ultimate lifetime and activity. Herein, we developed a facile approach for the synthesis of porous and hierarchical mono- or bi-metallic titanium nitride nanotubes (NTs), and this robust non-carbon material was used as the Pt support. The optimized catalyst (Pt/Ti0.9Ni0.1N NTs) demonstrated a mass activity of 0.78 A mgPt−1 and a specific activity of 1.3 mA cm−2 at 0.9 V (vs. RHE), which is roughly 3.6 times that of the commercial Pt/C catalyst. In particular, the catalyst exhibited excellent stability, such that the mass activity remained 3.2 times greater than that of pristine commercial Pt/C even after 15 000 continuous cycles at up to 1.2 V; in addition, the structure of the catalyst was perfectly maintained. The experimental data demonstrates that the hollow and porous structures, the strong metal-support interaction, and the synergistic effects derived from the nickel doping contribute to the improved performance and durability of the catalyst. This study paves the way for the rational synthesis of robust non-carbon catalysts that can be applied in a wide range of energy conversion processes.
研究领域:
材料科学
·
能源工程
·
催化化学
✓ 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）