LANGMUIR
·
2026
·
IF 4.4
Xuan Yang,Jing Ren,Tianjing Shi,Yongkang Lv,Rui-Peng Ren
Abstract Nitrogen-doped carbon materials derived from metal–organic framework (MOF) have been commonly regarded as promising metal-free electrocatalysts for the oxygen reduction reaction (ORR). However, their performance is severely limited by nanoparticle agglomeration-induced sluggish mass transfer, insufficient ORR intermediate adsorption regulation by sole N doping, and structural damage from excessive heteroatom doping. Herein, we report a mesoscopic superstructure engineering strategy to fabricate moderately nitrogen–oxygen codoping MOF-derived carbon sphere superstructures (N/O-CNS) for high-performance ORR. A three-dimensional (3D) spherical MOF superstructure precursor was first constructed via urea-induced self-assembly of one-dimensional (1D) rod-like Zn-MOF-74, followed by one-step controlled pyrolysis to preserve the 3D hierarchical architecture and achieve uniform nitrogen–oxygen doping. The 3D superstructure provides abundant accessible catalytic centers and accelerated mass/electron transport rates. Density functional theory (DFT) calculations verify that, compared with sole N doping, nitrogen–oxygen codoping further optimizes the adsorption energy of the rate-determining *OOH intermediate and lowers the ORR reaction energy barrier. Regulated pyrolysis enables continuous tuning of nitrogen–oxygen codoping content and the graphitization degree of the carbon matrix, achieving a favorable trade-off among catalytic site population, charge transport efficiency, and structural integrity. Notably, the optimized N/O-CNS-1000 with the lowest doping content among all samples exhibits exceptional ORR activity in alkaline electrolyte, with an onset potential of 0.98 V and a half-wave potential (E1/2) of 0.83 V, outperforming commercial Pt/C. When assembled into rechargeable Zinc-air batteries (ZABs), the N/O-CNS cathode achieves a maximum power density of 140.55 mW cm–2 and good cycling lifespan of over 750 h.
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DOI
高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
·
2019
·
IF 4.197
Haoran Yuan,Huibing Chen,Denian Li,Lifang Deng,Jian Chen,Yukun Fan,Mingyang He,Fuan Sun
Although oxygen reduction reaction (ORR) plays a key role in the cathodic part of many emerging energy conversion devices, it has naturally suffered from sluggish kinetics and high overpotential. We here report the facile synthesis of Fe-N co-doped carbon with a hierarchical porosity and in-situ formed graphene from biomass tar using urea as the nitrogen dopant, and FeCl 3 as the porogen, catalyst, and Fe dopant. This exhibited an ORR catalytic activity comparable to that of a Pt/C catalyst in relation to its onset potential, limited diffusion current, and stability under an alkaline condition. It was found that the excellent catalytic performance should have originated from its large specific surface area, abundant active centers, and long-term conductive network. This renewable non-noble-metal catalyst may serve as an appropriate alternative to conventional noble catalysts in ORR-based techniques, and will also encourage investigations on the use of biomass tar for advanced materials toward various ends.
研究领域:
材料科学
·
能量转换
·
电催化
·
可持续化学
·
纳米材料
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DOI
高影响因子
Scientific Reports
·
2017
·Vol. 7
·期 1
·1-11
·
IF 4.259
Zhang Qian,Zhang Yihe,Meng Zilin,Tong Wangshu,Yu Xuelian,An Qi
Photocatalysis is a promising strategy to address the global environmental and energy challenges. However, the studies on the application of the photocatalytically degraded dye-polluted water and the multi-purpose use of one type of catalyst have remained sparse. In this report, we try to demonstrate a concept of multiple and cyclic application of materials and resources in environmentally relevant catalyst reactions. A magnetic composite catalyst prepared from exfoliated titania nanosheets, graphene, the magnetic iron oxide nanoparticles, and a polyelectrolyte enabled such a cyclic application. The composite catalyst decomposed a methylene blue-polluted water under visible light, and then the catalyst was collected and removed from the treated water using a magnet. The photocatalytically treated water was then used to prepare the electrolyte in electrochemical reductive reactions and presented superior electrochemical performance compared with the dye-polluted water. The composite catalyst was once again used as the cathode catalyst in the electrochemical reaction. Each component in the composite catalyst was indispensable in its catalytic activity, but each component played different roles in the photochemical, magnetic recycling, and electrochemical processes. We expect the report inspire the study on the multi-functional catalyst and cyclic use of the catalytically cleaned water, which should contribute for the environmental and energy remedy from a novel perspective.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 9
·期 5
·2764-2774
·
IF 11.301
Yali Wang,Ruihui Gan,Hao Liu,Mahmut Dirican,Chengbiao Wei,Chang Ma,Jingli Shi,Xiangwu Zhang
The advancement of electrocatalysts using non-precious metals with excellent catalytic ability and durability for the oxygen reduction reaction (ORR) remains an enormous challenge. Transition metal–nitrogen–carbon (M–N–C) materials become target products with great development and application prospects for the ORR in new electrochemical energy storage and conversion devices. Herein, a simple preparation procedure of N-doped hierarchically porous carbon nanospheres loaded with Fe3O4/Fe2O3/Fe nanoparticles (Fe–CNSs–N) is developed by direct annealing of an Fe-doped quinone-amine polymer in an NH3/Ar atmosphere. Due to the integration of large specific surface area, hierarchically porous structure, and Fe3O4/Fe2O3/Fe nanoparticles, Fe–CNSs–N presents a half-wave potential of 0.835 V vs. RHE, which is 7 mV more positive than that of a commercial Pt/C catalyst in an alkaline medium. It also exhibits outstanding long-cycle durability as well as methanol endurance, superior to the Pt/C catalyst. Compared to the zinc–air battery based on Pt/C, the Fe–CNSs–N-based battery presents a higher open-circuit potential of 1.54 V, steadier discharge–charge cycle performance and an outstanding maximum power density of 106.8 mW cm−2. The excellent electrocatalytic performances make Fe–CNSs–N a promising substitute for Pt/C noble-metal catalysts in rechargeable Zn–air batteries.
研究领域:
材料科学
·
能源化学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Dahuan Li,Yongfang Qu,Xuejun Liu,Cuiping Zhai,Yong Liu
It is of significant importance to construct the low-cost, efficient, and stable carbon-based non-noble metal to replace the noble metal electrocatalyst for oxygen reduction reaction in both alkaline and acidic media. In this work, a straightforward and cost-efficient strategy is reported to synthesize the Fe–N co-doped open-porous carbon materials with three-dimensional (3D) carbon networks structure, high surface areas and multiple actives sites including iron carbide nanoparticles , pyridinic N, and graphitic N using a new kind of Fe-Imace coordinated complex as the precursor and melamine as nitrogen sources by direct pyrolysis . The obtained Fe– N –C 900 catalyst shows excellent oxygen reduction performance in both alkaline (E onset , 1.014 vs. RHE) and acidic (E onset , 0.982 V vs. RHE) media, which are better than those of the Pt/C in alkaline (E onset , 0.986 vs. RHE) and acidic media (E onset , 0.979 V vs. RHE). Even more important, the stability and methanol tolerance of the Fe–N–C 900 catalyst are much better than that of the Pt/C catalyst in both alkaline and acidic media. All the results demonstrate that the present facile and universal one-step pyrolytic strategy can be used to synthesize catalyst materials as one of the superior non-precious cathode electrocatalysts for fuel cells.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Jiayu An,Wenjun Jiang,Fuwei Zhuang,Yinhua Ma,Su Zhan,Feng Zhou
Utilizing photocatalytic technology to achieve efficient production of H2O2 is a hot topic. Here, we synthesized a photocatalytic material with a strong built-in electric field, namely, Pym-CN, through a hydrothermal-assisted thermal polymerization strategy, which effectively promotes the separation and transfer of photoinduced charge carriers. A pyrimidine ring was successfully introduced into the heptazine structure unit of Pym-CN, which leads to electron aggregation at N═C–N, benefiting for enhancing the strong sorption and activation capabilities of oxygen. Under the condition of visible light wavelength greater than 400 nm (λ > 400 nm), the H2O2 production rate of Pym-CN (2622.5 μmol/L/h) is 7.6 times that of the BCN. A detailed investigation of the reaction mechanism revealed that Pym-CN follows a two-step continuous process of single-electron oxygen reduction reaction (ORR). This work elucidates the application prospects of the donor–acceptor (D–A) structure with a strong built-in electric field in the field of efficient photocatalytic production of H2O2.
研究领域:
材料科学
·
光催化
·
可再生能源
·
化学工程
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Ya-Nan Sun,Jinqin Yang,Xuesong Ding,Wenyan Ji,Aleksander Jaworski,Niklas Hedin,Bao-Hang Han
High-efficient bifunctional catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are critical to the practical application of zinc–air batteries. Herein, a comprehensive investigation on the synergetic contribution of nitrogen (N) and fluorine (F) species in porous carbon for ORR/OER catalyses is firstly conducted. The metal-free N, F co-doped porous carbon (NFPC) possesses appealing catalytic activities in zinc–air batteries and is superior to many other catalysts. Combined with the careful exploration of N and F dopants, seventeen optimized carbon cluster structures with all possible co-doping of N and F species are considered for density functional theory calculations. It can be inferred that the F doping with graphitic and pyridinic N triggers active paramagnetic centers. The co-doping of covalent F and graphitic N especially gives the lowest free energy barrier for both ORR/OER, which could account for the notable performance of NFPC catalysts in zinc–air batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
催化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jing Li,Xiyu He,Yunzhu Du,Min Jiang,Qiaodan Hu,Jiewei Yin,Fan Yang,Junliang Zhang
Co/Mn-based spinel oxides are promising electrocatalysts for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), however, it is challenging to achieve high activities for ORR and OER simultaneously in one composition. Here, we report Co 2 MnO 4 (C2M) with Mn-rich surfaces and abundant twin defects synthesized by a simple coprecipitation and annealing route, which exhibits excellent ORR activity (half-wave potential E 1/2 = 0.830 V), long ORR durability (91% current retained after 12 h-chronoamperometry test at 0.45 V vs. RHE) and a low Δ E = 0.767 V between E 1/2 and E 10 mA/cm 2 in alkaline electrolyte, which enables its excellent performances in rechargeable Zn-air batteries showing a high peak energy density of 136 mW/cm 2 and a large specific capacity of 809.4 mAh/g Zn . Combining comprehensive experimental investigations and DFT simulations, we reveal that the Mn-rich surfaces benefit bridge adsorption of O 2 to promote the 4-electron reaction pathway in ORR, and the mixed site occupancy in the crystal structure induces Mn/Co-O orbital hybridizations to form an impurity energy level in the band gap to facilitate charge transfer. Furthermore, the bifunctional performance and the ORR durability can be further enhanced by acid treatment to show a lower Δ E = 0.750 V and to retain 98.5% ORR current in 12 h. This work provides not only a promising bifunctional electrocatalyst but also a new perspective of exploring simple synthesis method suitable for mass-producible electrocatalysts with highly active surfaces.
研究领域:
电化学
·
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Kun Liu,Yujing Ling,Xianglong Guan,Ke Hu,Angli Zhang,Kaiqi Liu,Haoyi Li,Guangnian Xu,Xu-Cheng Fu
The commercialization of magnesia-air batteries (Mg-air) necessitates the development of highly efficient, cost-effective, and durable electrocatalysts for oxygen reduction reaction (ORR), replacing expensive and unstable precious metal electrocatalysts. A hard template-assisted synthesis of FeCo nanoparticles immobilized on N-doped porous carbon (Fe-Co-C-N) for the ORR is reported. The half-wave potential of Fe-Co-C-N for ORR (E1/2=0.88 V vs. RHE) is elevated by 40 mV compared to that of 20 wt% Pt/C (E1/2=0.84 vs. RHE). The catalyst exhibits exceptional catalytic performance and remarkable stability. The discharge voltage of the Mg-air battery, utilizing Fe-Co-C-N as the cathode catalyst (1.29 V), surpasses that of the battery employing 20 wt% Pt/C as the cathode catalyst (1.28 V). The Mg-air battery with Fe-Co-C-N as the cathode catalyst exhibited excellent discharge stability and maintained a stable discharge for over 200 hours. The present study offers valuable insights into the structural design and regulatory mechanisms governing the performance of M-N-C catalysts in Mg-air batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yipu Xu,Wenru Zhao,Rui Chen,He Li,Xinyu Liu,Peiran Wu,Hui Yu,Jiansong Wang,Liu-Liu Shen,Gui-Rong Zhang,Donghai Mei
Zeolitic imidazolate frameworks (ZIFs) are widely explored as precursors for constructing electrocatalysts for the oxygen reduction reaction (ORR). However, most studies convert these frameworks into metal-nitrogen-carbon (M-N-C) catalysts via pyrolysis, a process that often compromises their structure integrity and coordination precision. Herein, it is demonstrated that ZIF-67 can serve directly as a highly-active molecular catalyst for ORR. By applying ball-milling to enhance cobalt sites exposure, the optimized ZIF-67 exhibits exceptional ORR activity in alkaline media. Combined spectroscopic and theoretical analyses reveal that this remarkable activity stems from coordinatively unsaturated Co-N 4-x sites, which transform into Co-N 4-x (OH) moieties under reaction conditions, thereby facilitating oxygen adsorption and activation. Furthermore, mild thermal treatment (≤500 °C) enhances the proportion of Co-N 4-x sites up to 48%, as confirmed by X-ray absorption spectroscopy, achieving ORR activity rivals or even exceeds conventional pyrolyzed M-N-C catalysts. This study unlocks the potential of ZIFs as active molecular electrocatalysts upon mild thermal treatment, providing a scalable and efficient strategy for optimizing ZIFs for catalytic applications while preserving their structural precision.
研究领域:
材料科学
·
电化学
·
催化
·
纳米技术
·
无机化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Qichao Chen,Chengjie Lu,Boyu Ping,Guiyang Li,Jiayi Chen,ZhengMing Sun,Yuanjian Zhang,Qiushi Ruan,Li Tao
Scalable solar-driven H 2 O 2 evolution from water holds great promise for industrial applications. Efficient H 2 O 2 generation relies on excellent spatial charge separation but simultaneously suffers from severe surface H 2 O 2 backreaction, which becomes a bottleneck for scalable H 2 O 2 evolution. Herein, a hydroxyl-induced carbon nitride (CN) homojunction coherently optimizes the bulk charge separation and suppresses surface backreaction. Surface hydroxyls provide extra electron accommodation bands for electron extraction from the bulk to the surface which are visually observed with KPFM and rationalized by DFT calculations. 2e - oxygen reduction reaction (ORR) kinetic became more favorable than 4e - ORR in the presence of hydroxyl, showing suppressed H 2 O 2 decomposition. This homojunction achieves a 4.5-fold improvement in H 2 O 2 production compared to pristine CN, and an apparent quantum yield (AQY) of 2.1 % at 500 nm in water. This work demonstrates a strategy for coherently improving spatial charge separation and surface reaction kinetics, which is applicable for various photocatalytic reactions.
研究领域:
材料科学
·
光催化
·
可再生能源
·
表面化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Xiao-ran Wen,Xue-wei Wang,Ke Ma,You-lin Chen,Chang Yu,Zhihao Yuan
Mullite oxides have been studied for decades as oxygen reduction reaction (ORR) electrocatalysts because of their flexible and tunable electronic structures. In this work, a larger radius La was used to replace Sm to synthesize a series of nanorod-shaped SmxLa1–xMn2O5 catalysts by a two-step hydrothermal method. Compared with SmMn2O5, Sm0.7La0.3Mn2O5 has a higher half-wave potential (0.83 V vs reversible hydrogen electrode), which exhibits excellent ORR electrocatalytic activity in alkaline media. Meanwhile, Sm0.7La0.3Mn2O5 shows better ORR stability, higher electron transfer number, and lower hydrogen peroxide yield. The excellent electrocatalytic activity is mainly owing to that the introduction of La changes the bond length of Mn–O, thereby increasing the amount of Mn3+. The elongated nanorods increase the specific surface area of the sample and exhibit more active sites on the reaction surface. Furthermore, rechargeable zinc–air batteries made of Sm0.7La0.3Mn2O5 not only have a high power density (147.1 mW cm–2), but exhibit excellent cycling stability in long-term charge–discharge tests over 800 h. This work not only provides a series of low-cost and highly active electrochemical catalysts for zinc–air batteries, but also provides a convenient and effective method for the wide and practical application of zinc–air batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）