Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Liu Cong,Mei Bingbao,Shi Zhaoping,Jiang Zheng,Ge Junjie,Xing Wei,Song Ping,Xu Weilin
Heterogeneous nano-electrocatalysts doped with nonmetal atoms have been studied extensively based on the so-called dopant-based active sites, while little attention has been paid to the stability of these dopants under working conditions. In this work, we reveal significantly, when the redox working potential is too low negatively or too high positively, the active sites based on these dopants actually tend to collapse. It means that some previously observed “remarkable catalytic performance” actually originated from some unknown active sites formed in situ. Take the Bi-F for the CO 2 RR as an example, results show that the observed remarkable activity and stability were not directly from F-based active sites, but the defective Bi sites formed in situ after the dopant leaching. Such a fact is unveiled from several heteroatom-doped nanocatalysts for four typical reactions (CO 2 RR, HER, ORR, and OER). This work provides insight into the role of dopants in electrocatalysis.
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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DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 9
·090514
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IF 4.316
Xiaochao Liu,Siyuan Peng,Xiaoxiao Li,Chao Liu,Jinming Zeng,Xiaopeng Qi,Tongxiang Liang
The development of low-cost, high catalytic activity oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) electrocatalysts is the key to promoting the development of zinc-air batteries. In this paper, a simple one-step pyrolysis method was used to successfully synthesize a binary FeCo–Co/NC catalyst with FeCo and Co nanoparticles encapsulated in N-doped carbon nanotubes. This structure exhibits great characteristics: it has a variety of active species (FeCo, Co, NC), and there is close combination between these active species (FeCo, Co, NC). Electrochemical studies have shown that the initial potential of FeCo–Co/NC during ORR process is 0.93 V, the half-wave potential is 0.808 V, and the limiting current density is 4.94 mA cm−2. In the OER process, at an anode current density of 10 mA cm−2, an overpotential of only 353 mV is shown; a lower Tafel slope and good durability are also observed. Moreover, the zinc-air battery in preparation can be cycled for as long as 2000 times. This provides a new method for the preparation of high-efficiency dual-function electrocatalysts for OER and ORR.
研究领域:
材料科学
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电化学
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能源存储与转换
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
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2025
·
IF 14.9
Juan Luo,Qing Li,Feng Liu,Jingjing Huang,Hao Cui,Yuke Gu,Meihuan Liu,Pengfei Tan,Jun Pan
Overcoming kinetic limitations in the acidic oxygen reduction reaction (ORR) demands Pt-based catalysts with optimized surface adsorption. Herein, we engineer hierarchical PtPd dendrite nanocrystals (PtPd NDs) featuring precisely tailored asymmetric sites and high-index facets (HIFs) to overcome the kinetic limitations in acidic media. Controlled Pd incorporation disrupts symmetry of the single-oriented crystal plane, generating inhomogeneous strain and promoting HIFs exposure. This synergistic structural engineering optimizes the adsorption/desorption of oxygen-containing intermediates, significantly accelerating ORR kinetics. Consequently, PtPd NDs deliver exceptional mass activity (MA = 1.37 A mg Pt −1 , 11.42 times higher than Pt/C) and remarkable stability (83.9% MA retention after durability testing). In H 2 -Air fuel cells, PtPd NDs also achieve higher peak power density versus Pt/C cathodes. In situ synchrotron radiation infrared spectroscopy and theoretical studies reveal that the synergistic effect between asymmetric sites and HIFs stimulates the strain field and causes a downward shift in the d -band center, thereby lowering the *OOH formation barrier and weakening intermediate adsorption, directly boosting the ORR performance. This work underscores the critical role of facet and site engineering in designing high-performance fuel cell electrocatalysts.
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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纳米技术
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能量转换
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DOI
高影响因子
MOLECULES
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2021
·Vol. 26
·期 21
·6672
·
IF 4.412
Syed Shoaib Ahmad Shah,Tayyaba Najam,Costas Molochas,Muhammad Altaf Nazir,Angeliki Brouzgou,Muhammad Sufyan Javed,Aziz ur Rehman,Panagiotis Tsiakaras
Heteroatom doping is considered an efficient strategy when tuning the electronic and structural modulation of catalysts to achieve improved performance towards renewable energy applications. Herein, we synthesized a series of carbon-based hierarchical nanostructures through the controlled pyrolysis of Co-MOF (metal organic framework) precursors followed by in situ phosphidation. Two kinds of catalysts were prepared: metal nanoparticles embedded in carbon nanotubes, and metal nanoparticles dispersed on the carbon surface. The results proved that the metal nanoparticles embedded in carbon nanotubes exhibit enhanced ORR electrocatalytic performance, owed to the enriched catalytic sites and the mass transfer facilitating channels provided by the hierarchical porous structure of the carbon nanotubes. Furthermore, the phosphidation of the metal nanoparticles embedded in carbon nanotubes (P-Co-CNTs) increases the surface area and porosity, resulting in faster electron transfer, greater conductivity, and lower charge transfer resistance towards ORR pathways. The P-Co-CNT catalyst shows a half-wave potential of 0.887 V, a Tafel slope of 67 mV dec−1, and robust stability, which are comparatively better than the precious metal catalyst (Pt/C). Conclusively, this study delivers a novel path for designing multiple crystal phases with improved catalytic performance for energy devices.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Hongguan Li,Jing Wang,Ruijuan Qi,Yongfeng Hu,Jing Zhang,Hongbin Zhao,Jiujun Zhang,Yufeng Zhao
Charge and spin manipulations of electrons are considered to be of great significance in boosting the catalytic activity of M N C electrocatalysts. However, to the best of our knowledge, most current studies focus only on the charge engineering, the interplay between spin and charge is not well understood, and the simultaneous manipulation of both charge and spin remains challenging. Herein, we show that the cooperative interplay between charge itineration and spin-polarization of electrons has a profound impact on the catalytic behavior through density functional theory (DFT) calculations for the first time. Following this concept, we report a Fe-Ni atomic pair as a superior bifunctional catalyst for high performance ORR and OER, with a very small potential difference (ΔE) of 0.691 V. We confirm that the coexistence of Fe 3d itinerant charge and moderate spin polarization (magnetic moment: 1.48 μ B ) is responsible for the superior functional catalytic activity for the Fe Ni atomic pairs.
研究领域:
电催化
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材料化学
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物理化学
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纳米催化
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能源材料
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计算化学
✓ 已验证
DOI
高影响因子
Materials Chemistry Frontiers
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2022
·Vol. 6
·期 21
·3213-3224
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IF 8.683
Wenfang Miao,Feirong Huang,Xiaochen Shen,Shaopeng Li,Xingru Cao,Xuefeng Zhang,Jieyi Yu,Xinglong Dong
The development of high-efficiency, stable, and low-cost Fe–N–C electrocatalysts for the oxygen reduction reaction (ORR) has attracted considerable attention. Herein, a stable atomically dispersed Fe–Nx-based catalyst was synthesized from a hierarchical structure involving carbon nanofiber (CNF)-supported zeolitic-imidazolate-framework-8 (ZIF-8) encapsulated Fe–Phen complex ((Fe,N)-ZIF-8/CNFs). The Fe–Nx–CNFs obtained from the pyrolysis of (Fe,N)-ZIF-8/CNFs showed a good hierarchical multi-layer structure. The natural network structure of the carbon nanofibers serves as a matrix to uniformly distribute the ZIF-8 particles, and the Fe–Nx sites derived from the Fe–Phen complex were uniformly distributed in ZIF-8 particles. It exhibits excellent ORR performance with a high half-wave potential of 0.875 V (vs. RHE), which was 55 mV higher than that of the commercial Pt/C catalyst. In addition, density functional theory (DFT) calculations on the catalyst further revealed the origin of the ORR activity via a 4e− pathway from the precise local coordination of FeN4 sites.
研究领域:
材料科学
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电化学
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催化化学
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纳米技术
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能源化学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
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2021
·Vol. 105
·期 4
·2690-2701
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IF 3.784
Lu Zou,Zhao Lu,Ziling Wang,Bo Chi,Jian Pu
Developing high-efficiency and cost-effective bifunctional electrocatalysts toward the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is an urgent issue for the oxygen-based electrochemical devices. Herein, an interface engineering concept has been proposed to achieve high-performance Ag–PBSC (Ag–PrBa 0.5 Sr 0.5 Co 2 O 5+δ ) heterostructure nanofibers catalyst. Benefiting from the significant ligand action and interparticle cooperation of exsolved Ag NPs and PBSC double perovskite, ORR/OER catalytic kinetics have been successfully boosted. In details, the PBSC double perovskite possessing abundant oxygen vacancies can provide oxygen channels and facilitate the transfer of electrons and oxygen. The embedded Ag NPs can deliver superior catalytic durability for the heterostructure interface. As expected, the as-synthesized Ag-PBSC heterostructure catalyst performs a favorable electrochemical performance in the oxygen-based applications. In alkaline media, the catalyst exhibits an excellent activity for ORR ( E onset : 0.88 V vs. RHE and E 1/2 : 0.72 V vs. RHE) and OER (1.67 V at 10 mA cm –2 ). When adopting the Ag–PBSC heterostructure catalyst in LOBs, the corresponding battery provides an outperforming capacity performance (13 000 mAh g –1 ), low discharge–charge polarization (1.37 V), and considerable cycling performance (128 cycles at the restricted capacity of 3 000 mAh g –1 and 400 mA g –1 ). Apparently, the work described here confirms that the interface engineering of perovskites can open up opportunities to develop highly active and durable heterostructure electrocatalysts for multitudinous oxygen-based electrochemical applications.
研究领域:
材料科学
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电化学
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能源存储与转换
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
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2026
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IF 8.4
Ruite Gu,Tingyu Yan,Zeyu Hao,Huanlu Tu,Shansheng Yu,Xiaoying Hu,Hongwei Tian
The preparation of highly efficient, stable, and cost-effective catalysts to address the complex oxygen reduction reaction (ORR) in zinc-air batteries remains a significant challenge. Herein, a surface modification strategy is employed to uniformly encapsulate an Fe-N-C matrix with cobalt-coordinated conjugated organic polymers containing Schiff base structures, successfully yielding a highly active CB(cobalt-coordinated Schiff-base polymer)@Fe-N-C composite catalyst with coexisting cobalt coordination polymers and iron-nitrogen-carbon structures. In alkaline electrolytes, the CB@Fe-N-C catalyst exhibits outstanding catalytic activity (E 1/2 = 0.93 V) and stability, which are attributed to its highly conductive, structurally stable composite architecture with abundant active sites. In a zinc-air battery (ZAB), CB@Fe-N-C exhibits remarkable power density, surpassing the Pt/C benchmark. This work offers an effective synthetic strategy for preparing electrocatalysts with excellent ORR performance in zinc-air batteries.
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DOI
高影响因子
Materials
·
2025
·Vol. 18
·期 8
·1786
·
IF 3.2
Xu Wang,Nan Wang,Kunpeng Liu,Meinan Yang,Ruiyong Zhang,Sikandar Khan,Jinhui Pang,Jizhou Duan,Baorong Hou,Wolfgang Sand
Marine biofouling causes significant economic losses, and conventional antifouling methods are often associated with environmental pollution. Hydrogen peroxide (H2O2), as a clean energy source, has gained increasing attention in recent years. Meanwhile, electrocatalytic 2e−oxygen reduction reaction (ORR) for H2O2production has received growing interest. However, the majority of current studies are conducted on acidic or alkaline electrolytes, and research on 2e−ORR in neutral NaCl solutions remains rare. Here, a bimetallic Zn-Cd zeolitic imidazolate framework (ZnCd-ZIF) is rationally designed to achieve chloride-resistant 2e−ORR catalysis under simulated seawater conditions (pH 7.5, 3.5% Cl−). Experimental results demonstrate that the ZnCd-ZIF catalyst exhibits an exceptional H2O2selectivity of 70% at 0.3 VRHE, surpassing monometallic Zn-ZIF (60%) and Cd-ZIF (50%). Notably, H2O2production reaches 120 mmol g−1in a Cl−-containing neutral electrolyte, exhibiting strong resistance to structural corrosion and Cl−poisoning. This work not only pioneers an effective strategy for designing ORR catalysts adapted to marine environments but also advances the practical implementation of seawater-based electrochemical H2O2synthesis.
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Qing Chen,Ling Shi,Guiping Xu,Maocong Hu,Mao Peng,Zhenhua Yao
The development of low-cost and efficient bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of importance for the commercialization of green and sustainable energy conversion devices. In this work, noble metal-free XFeCoNiCu (X = Cr, Mg, and Mn) high entropy alloys were prepared with a facile pyrolytic reduction approach while the structure and composition were characterized by XRD, ICP-OES, TEM, HRTEM, and XPS. The prepared quinary alloys demonstrated excellent activity and stability for both ORR and OER, which was even superior to that of commercial Pt/C and RuO₂. Moreover, all three catalysts exhibited considerable potential for bifunctional catalysis, with a ΔE gap of 0.659 V for CrFeCoNiCu, a ΔE gap of 0.692 V for MnFeCoNiCu, and a ΔE gap of 0.727 V for MgFeCoNiCu, which was much better than that of the Pt/C+RuO 2 combination (0.723 V). The superior performance was further revealed by Density Functional Theory (DFT) calculations with projection density of states (PDOS) and free energy change. The strategy proposed in this study provides an economical approach to design and develop bifunctional electrocatalysts with exceptional performance.
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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产品关联
DOI
高影响因子
CARBON
·
2020
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IF 8.821
Xingwei Zhou,Xin Liu,Jiahao Zhang,Cai Zhang,Seung Jo Yoo,Jin-Gyu Kim,Xianyu Chu,Chao Song,Peng Wang,Zhenzhen Zhao,Dabing Li,Wei Zhang,Weitao Zheng
Preventing agglomeration and corrosion of metal electrocatalysts at nanoscale is crucial for electrochemical energy conversion, such as fuel cell and overall water splitting , where all the oxygen evolution reaction (OER), hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) are the core. Herein, an effective strategy is developed for preparing multifunctional self-supporting electrocatalysts with uniformly distributed cobalt nanoparticles and clusters. Benefiting from good electrical conductivity and multiple active sites, the trifunctional self-supporting catalyst free from stacking and aggregating exhibits excellent OER and HER activities with an overpotential of 270 and 110 mV to obtain a current density of 10 mA cm −2 in alkaline media . The ORR performance was tested in 0.1 M KOH solution with a half-wave potential of ∼0.80 V and a limiting current density of ∼ −4.8 mA cm −2 . Our finding provides an opportunity for the rational design of multifunctional and highly-efficient self-supporting electrocatalysts towards the integration of electrochemical energy conversion.
研究领域:
材料科学
·
电化学能源转换
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry C
·
2022
·
IF 4.177
Weifeng Su,Ning Yan,Fan Liu,Zigeng Liu,Guangqi Zhu,Songrui Wang,Xingjiang Liu,Wei Wang
The attenuation process of the oxygen reduction reaction (ORR) catalytic performance for Fe SAC@G catalysts under different discharging conditions, including KOH concentrations, solution temperatures, and discharging potentials, was investigated by electrochemical measurements. The ORR catalytic activity attenuation resulting from the change in KOH concentration and temperature becomes apparent in a negative discharging potential range and elevated discharging temperature. In addition, the more negative discharging potential significantly causes the ORR catalytic activity attenuation. Scanning electron microscopy (SEM), energy-dispersive spectrometry (EDS), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy analyses indicate that, with the prolongation of the discharge time, the nanocolumns of the as-prepared catalyst gradually dissolve, while a flowerlike discharge byproduct composed of elements C and N keeps growing on the surface of the catalyst. The weakest Fe–N bonds first break, resulting in the attenuation of the ORR catalytical performance. Then, the weak C–Cunit bonds connecting the structural units of the catalysts break, leading to the gradual collapse in the structure of the catalysts. The Fe–N4 coordination structure gradually transforms into Fe–N3, Fe–N2, and Fe–N coordination structures. Based on the analyses combined with the density functional theory (DFT) calculations of bond strength, a discharge attenuation mechanism of the structural collapse of the catalyst for the formation of the discharge byproduct with ring structure is proposed.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
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