JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2017
·Vol. 21
·期 6
·1639-1651
·
IF 2.316
He Hongyun,Wang Min,Zhang Yan,Zhao Jinsheng
A novel composite formed between nitrogen-rich soluble conjugated polymer and carbon was prepared and evaluated as a candidate for oxygen reduction reaction (ORR) catalyst, and the composite was designated as PBBDP/C. The complexation between copper ion (II) and PBBDP/C formed another catalyst, named Cu-PBBDP/C. Electrochemical tests including cyclic voltammetry (CV), linear sweep voltammetry (LSV), and rotating ring disk electrode (RRDE) were used for the characterization of the ORR activities of the catalysts. The measurements showed that both of the catalysts showed considerable stability and apparent ORR activities, and the ORR activity of Cu-PBBDP/C was much higher than that of PBBDP/C. For digging into the exact ORR mechanisms, the rate constants of possible ORR pathways were calculated as analyzed for both catalysts. For PBBDP/C catalyst, the result indicated that oxygen was reduced through two parallel routes, the four-electron pathway and the two-electron pathway taking H 2 O 2 as the intermediate product. For Cu-PBBDP/C catalyst, the ORR was via a four-electron transfer-dominant process. In this case, the Cu-N
x
group is active sites for the direct reduction of oxygen to water.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2017
·
IF 4.233
Wenbei Zhang,Tianlu Cui,Lingyun Yang,Chao Zhang,Ming Cai,Sai Sun,Yefeng Yao,Xiaodong Zhuang,Fan Zhang
Iron and nitrogen (Fe/N) co-doped porous carbons have already shown great potential as electrocatalysts for oxygen reduction reaction in alkaline media. However, it still remains a great challenge to finely integrate a hierarchical porous structure and Fe/N co-doping effect into one material at the same time. In this work, a rational design toward Fe/N-codoped hierarchical porous carbon spheres was developed by the formation of an iron-porphyrin-containing conjugated microporous polymer sphere with hollow structure (HCMP) through a silica sphere template directed condensation of pyrrole and 1,4-phthalaldehyde, then etched with NaOH, and treated with FeCl 2 . The resulting HCMP-Fe polymer was readily converted to a series of Fe/N co-doped hierarchical porous carbons (HPC-Fe/N-X, X = 700–900) upon pyrolysis at different temperatures and etching treatment. These porous carbons exhibit the high specific surface areas up to 518 m 2 g −1 and the contents of N and Fe up to 3.28 at.% and 0.85 wt.%, respectively. Benefiting from the high surface area, Fe/N co-doping character, HPC-Fe/N-700 exhibited excellent electrochemical catalytic performance for oxygen reduction reaction under alkaline condition (0.1 M KOH) with a low half-wave potential (0.84 V), a dominant four-electron transfer mechanism (n = 3.89 at 0.65 V), as well as a high diffusion limiting current density ( J L = 5.19 mA cm −2 ), comparable to those porous carbon-based ORR catalysts with excellent electrochemical performance.
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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2017
·
IF 3.582
Yingjie Chen,Shiben Liu,Liyan Yu,Qiuhong Liu,Yongtao Wang,Lifeng Dong
Nanoparticles with core–shell or hollow interiors have immense potential for catalysis. Herein, Ag@M x Fe 3− x O 4 (M = Co, Mn) core–shell nanoparticles were firstly synthesized through a seed-mediated method. These particles were then loaded onto carbon catalyst supports to form Ag@M x Fe 3− x O 4 /C. Then, hollow-M x Fe 3− x O 4 /C was prepared with the diffusion of Ag from Ag@M x Fe 3− x O 4 /C in saturated NaCl solution at room temperature . As a result, Ag@MnFe 2 O 4 /C demonstrates better oxygen reduction reaction (ORR) activity than Ag@CoFe 2 O 4 /C and other Ag@Mn x Fe 3− x O 4 /C with various Mn/Fe ratios. Moreover, Ag@MFe 2 O 4 /C shows superior ORR catalytic activities over hollow-MFe 2 O 4 /C, which can be due to electronic coupling between Ag core and MFe 2 O 4 shell. Furthermore, Ag@MnFe 2 O 4 /C catalysts demonstrate high durability for the ORR in alkaline media and insensitivity to methanol. These findings will provide helpful guidance for design and fabrication of carbon-supported core–shell catalysts for ORR in the future.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2016
·Vol. 163
·期 9
·H738
·
IF 3.014
Li Zhang,Han Wang,Hong Wang,Xiao-Peng Liu,Liang Su,Liang Yu,Ping Chen
Exploring the nonprecious metal catalysts for oxygen reduction with high activity and stability in acidic media is still a hard but extremely desirable work. Here, we proposed a bulk production of N, Fe-doped carbon nanospheres. The process involved a hydrothermal polymerization of m-phenylenediamine with FeCl3 as catalysts to catalyze the formation of poly(m-phenylenediamine) and annealing in NH3 atmosphere. The typical product has high surface area (1408 m2 g−1), big total pore volume (0.90 cm3 g−1) and a number of micropores. The typical product possesses the excellent activity for ORR, endurance and tolerance to methanol in acidic circumstance. This work has the merits of careful selection of poly(m-phenylenediamine) as precursor and NH3 etching to prepare the high-performance ORR catalysts in acidic electrolyte. The approach is simple, low-cost and readily scalable.
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 Applied Materials & Interfaces
·
2016
·
IF 7.145
Likai Wang,Zhenghua Tang,Wei Yan,Hongyu Yang,Qiannan Wang,Shaowei Chen
Porous carbon-supported gold nanoparticles of varied sizes were prepared using thiolate-capped molecular Au25, Au38, and Au144 nanoclusters as precursors. The organic capping ligands were removed by pyrolysis at controlled temperatures, resulting in good dispersion of gold nanoparticles within the porous carbons, although the nanoparticle sizes were somewhat larger than those of the respective nanocluster precursors. The resulting nanocomposites displayed apparent activity in the electroreduction of oxygen in alkaline solutions, which increased with decreasing nanoparticle dimensions. Among the series of samples tested, the nanocomposite prepared with Au25 nanoclusters displayed the best activity, as manifested by the positive onset potential at +0.95 V vs RHE, remarkable sustainable stability, and high numbers of electron transfer at (3.60–3.92) at potentials from +0.50 to +0.80 V. The performance is comparable to that of commercial 20 wt % Pt/C. The results demonstrated the unique feasibility of porous carbon-supported gold nanoparticles as high-efficiency ORR catalysts.
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
·
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
·
2015
·Vol. 5
·期 125
·103421-103427
·
IF 3.84
Likai Wang,Zhenghua Tang,Xiaojun Liu,Wenhan Niu,Kai Zhou,Hongyu Yang,Weijia Zhou,Ligui Li,Shaowei Chen
Unlike bulk gold, gold nanoparticles (AuNPs) have been found to exhibit apparent electrocatalytic activity for oxygen reduction reaction (ORR). In this work, glutathione-capped AuNPs of ca. 4 nm in diameter were prepared by a wet chemical method and embedded into a mesoporous carbon matrix synthesized by using an SBA-15 amorphous silica template. Pyrolysis at elevated temperatures led to removal of the organic capping ligands and the formation of ordered mesoporous carbons loaded with a selected amount of AuNPs which exhibited no apparent agglomeration. The obtained nanocomposites exhibited apparent ORR activity in alkaline media, and the sample with 20 wt% AuNPs stood out as the best among the series, within the context of onset potential, kinetic current density and stability, in comparison with AuNPs alone, ordered mesoporous carbons, and commercial Pt/C catalysts. The remarkable performance was ascribed to the intimate interactions between the AuNPs and mesoporous carbons that facilitated fast electron transfer and rapid mass transport. This is the first time that ordered mesoporous carbons were employed to support AuNPs as ORR catalysts. The strategy may be exploited to prepare a wide range of electrocatalysts based on mesoporous carbons-supported metal nanoparticles with extraordinary reactivity and enhanced stability for ORR.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2016
·Vol. 12
·期 10
·1295-1301
·
IF 8.315
Long Liu,Xianfeng Yang,Na Ma,Haitao Liu,Yanzhi Xia,Chengmeng Chen,Dongjiang Yang,Xiangdong Yao
Graphical A simple and scalable synthesis of a 3D Fe 2 N-based nanoaerogel is reported with superior oxygen reduction reaction activity from waste seaweed biomass, addressed the growing energy scarcity. The merits are due to the synergistic effect of the 3D porous hybrid aerogel support with excellent electrical conductivity, convenient mass transport and O 2 adsorption, and core/shell structured Fe 2 N/N-doped amorphous carbon nanoparticles.
研究领域:
能源材料科学
·
环境科学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
IONICS
·
2021
·Vol. 27
·期 9
·3975-3985
·
IF 2.817
Wang Zhiyi,Wang Yutian,Tang Jingtao,Wang Kaizhao,Chen Tianyou,Wang Kaijun,Hu Jin
Among the currently studied nitrogen-doped Pt-C catalysts, the environmental friendliness of the nitrogen source and the stability of Pt-C catalysts for fuel cells are urgent issues to be solved. In this study, nitrogen-doped platinum-based catalyst (CSC/BP-Pt) with excellent stability for the ORR is prepared by a self-doping method based on chitosan (CS), a green biomass material with both nitrogen and carbon sources, in combination with conductive carbon black (BP2000). Finally, the N content of the catalyst is as high as 5.8 wt%, which is higher than most comparable catalysts (3–5 wt%). And electrochemical tests show that the CSC/BP-Pt electrochemical active surface area (ECSA) = 154.1 m 2 /g Pt , half-wave potential (E 1/2 = 0.85 V RHE ) has a better electrochemical performance than the commercial Pt/C (20 wt%), while the half-wave potential is reduced at 10,000 cycles of cyclic voltammetry with almost no attenuation (only 7 mVcompared to 31 mV of Pt/C). Besides, possible mechanisms to improve the activity and stability of CSC/BP-Pt are preliminarily proposed.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Meiying Yu,Yunfei Li,Xuepeng Chen,Xiaole Yuan,Nan Li,Weihua He,Yujie Feng,Jia Liu
Cathode membrane adding zinc phthalocyanine (ZnPc) is an efficient strategy to improve catalytic performance and antifouling properties. The maximum current density and the lowest charge transfer impedance of cathode membrane with the 0.07 g ZnPc (ZnPc-7) are 11.7 A m −2 and 5.3 Ω. The ZnPc-7 is also proven to be an excellent 4e − catalyst. The ZnPc-7+E (E is electric) produces the minimum total permeability decay rate and the lowest irreversible permeability attenuation rate under electric field, which are decreased by 19% and 64% than the control+E. The ZnPc enhances the antifouling performance and reproducible positive effect under electric field. The foregoing can be attributed to that ZnPc with superior conductivity produces rapid electrochemical response and stronger electrostatic repulsion force under electric field condition, thus reducing the membrane fouling . This work provides a simple strategy for the improvement of antifouling performance of filtration cathode membranes in microbial fuel cells .
研究领域:
环境科学
·
材料科学
·
微生物学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Fengxian Zhang,Ye Chen,Yang Liu,Xupo Liu,Shuyan Gao
Constructing highly efficient and durable non-noble metal modified carbon catalysts for oxygen reduction reaction (ORR) in the whole pH range is essential for energy conversion devices but still remains a challenge. Herein, the Fe/Fe 3 C nanoparticles and Fe-N X species anchored on the interconnected mesoporous carbon materials are fabricated through an economical and facile template-assisted polymerization-pyrolysis strategy. The catalyst exhibits unique features with the electronic interaction between Fe/Fe 3 C and Fe−N X , large specific surface area and high mesoporous structure as well as nitrogen doping in porous carbon skeletons, which can effectively catalyze ORR over the full pH range. In an alkaline electrolyte , the optimized catalyst displays favorable ORR performance with positive onset potential ( E onset = 0.91 V), half-wave potential ( E 1/2 = 0.83 V), long-term cycles stability and methanol tolerance, exceeding those for the commercial Pt/C. Furthermore, the prepared catalyst could be directly assembled into the alkaline Zn−air battery that exhibits the open-circuit voltage of 1.44 V, high power density of 96.0 mW cm −2 and long-term durability. Therefore, the template-assisted polymerization-pyrolysis strategy provides a promising route for designing high-performance non-noble metal decorated ORR electrocatalysts .
研究领域:
材料科学
·
电化学
·
能源转换技术
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Science
·
2022
·Vol. 16
·期 1
·210-221
·
IF 39.714
Hongyuan Yang,Jie Wu,Zhengran Chen,Kai Zou,Ruihong Liang,Zhenhui Kang,Prashanth W. Menezes,Ziliang Chen
Physical field modulation has been regarded as a promising approach to boost the performance of various electrocatalysts and has recently received notable attention. However, such a technique by coupling an external field to controllably enable efficient and green electrosynthesis of hydrogen peroxide (H2O2) through a 2e− oxygen reduction reaction (ORR) has not been perceived so far. In order to address the feasibility of this method, a controllable piezoelectric strategy based on the response of intrinsic electric domains to the stimulation of fluid mechanical force was exploited effectively to induce local electric fields on the polarized ceramic catalyst surface during the dynamic ORR. By adjusting the polarization degree of ceramic catalysts, the strength of the local electric field could be accordingly modulated, thus tuning the coverage of OH− ions on the catalyst surface which is beneficial for optimizing the binding strength towards oxygen-containing intermediates and alleviating the disproportionation of the peroxide product.
研究领域:
材料科学
·
电化学
·
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）