CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Peng Wei,Xiaogang Li,Zhimin He,Xueping Sun,Qirui Liang,Zhengying Wang,Chun Fang,Qing Li,Hui Yang,Jiantao Han,Yunhui Huang
The flexible design and construction of oxygen reduction reaction (ORR) catalysts with high activity, great stability, and superior cost efficiency are essential for metal-air batteries and fuel cells. Hollow carbon nanotubes (CNTs) are considered promising electrocatalysts owing to their outstanding thermal stability, robust chemical properties, and high specific surface area. Herein, a convenient and controllable solid-phase route is proposed for the preparation of porous nitrogen (N) and boron (B) co-doped carbon nanotubes (NBCNT) by using tubular polypyrrole (PPy) and sodium tetraphenylboron ((C 6 H 5 ) 4 BNa), in which (C 6 H 5 ) 4 BNa serves not only as a B source but also as a pore-forming agent that can help to regulate N configuration and expose more active sites. Due to the synergistic effects of porous one-dimensional hollow structure and the binary heteroatom doping, the optimized NBCNT catalyst demonstrates superior catalytic performance for ORR in both acidic and alkaline electrolytes. Moreover, Zn-air batteries are constructed based on the as-prepared catalysts, which reveal a high operating voltage (1.43 V) and peak power density (173.93 mW cm −2 ), further demonstrating a comparable electrocatalytic performance of the catalysts to commercial Pt/C catalyst. This work reveals a novel construction of high-efficiency and cost-effective metal-free catalysts for various energy conversion and storage technologies.
研究领域:
材料科学
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电化学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Yiyang Lin,Kang Liu,Kejun Chen,Yan Xu,Hongmei Li,Junhua Hu,Ying-Rui Lu,Ting-Shan Chan,Xiaoqing Qiu,Junwei Fu,Min Liu
Atomically dispersed FeN4 catalysts have been considered as potential materials to replace Pt-based catalysts for the oxygen reduction reaction (ORR), but they often suffer from sluggish O2 activation kinetics due to the symmetrical charge distribution. Herein, we introduce external N, including pyrrolic-N (PN) and graphitic-N (GN), as an electron acceptor near FeN4 to regulate its charge distribution and improve its ORR activity. Theoretical calculations reveal that introduction of PN evokes much enhanced electron redistribution and local electrical field on the Fe site compared with those observed with GN introduction and the pristine one. Synchrotron X-ray absorption spectroscopy and X-ray photoelectron spectroscopy validate the positive charge accumulation of Fe in the FeN4 site induced by introducing PN. Thus, the obtained FeN4-PN exhibits a great performance for ORR in 0.1 M KOH with a remarkable half-wave potential of 0.91 V versus reversible hydrogen electrode, as well as a Tafel slope of 58 mV decade–1. This work provides a guide to improve the catalytic performances of single-atom catalysts by introducing charge-redistribution sites.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2019
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IF 12.221
Mingxing Gong,Zhiping Deng,Dongdong Xiao,Lili Han,Tonghui Zhao,Yun Lu,Tao Shen,Xupo Liu,Ruoqian Lin,Ting Huang,Guangwen Zhou,Huolin Xin,Deli Wang
Developing highly active as well as durable oxygen reduction reaction (ORR) electrocatalysts are still imperative for clean and efficient energy conversion device, such as fuel cells and metal-air battery. For this purpose and maximize the utilization of noble Pt, we present here a facile, yet scalable strategy for the high-precise synthesis of 1-nm-thick Pt3Ni bimetallic alloy nanowires (Pt3Ni BANWs). The seed-mediated growth mechanism of Pt3Ni BANWs was identified subsequently. As expected, the Pt3Ni BANWs delivered enhanced mass activity (0.546 A mgPt–1, exceeding the 2020 target of DOE) in comparison to Pt nanowires assembly (Pt NWA, 0.098 A mgPt–1) and Pt/C (Pt, 0.135 A mgPt–1), because of the rational integration of multiple compositional and structural advantages. Moreover, the Pt3Ni BANWs displayed enhanced durability (37% MA retention) than Pt NWA and Pt after 50 000 potential cycles. All these results indicate that the ultrathin Pt3Ni BANWs are potential candidates for catalyzing ORR with acceptable activity and durability. The present work could not only provide a facile strategy but also a general guidance for the design of superb performance Pt-based nanowire catalysts for ORR.
研究领域:
材料科学
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电化学
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能源转换技术
✓ 已验证
产品关联
DOI
高影响因子
IONICS
·
2021
·Vol. 27
·期 9
·3975-3985
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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
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电化学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
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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
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材料科学
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微生物学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2019
·
IF 10.159
Shanshan Zeng,Fucong Lyu,Ligang Sun,Yawen Zhan,Fei-Xiang Ma,Jian Lu,Yang Yang Li
In this work, UiO-66-based metal–organic frameworks are investigated as an oxygen reduction reaction (ORR) catalyst for the first time. UiO-66-NO2 is solvothermally grown on the surface of cobalt phthalocyanine-anchored carbon nanotube (CoCNT) surface, serving as an oxygen “pump” to accelerate the oxygen reduction reaction (ORR). The UiO-66-NO2-attached CoCNT (UiO-66-NO2@CoCNT) exhibits superior electrochemical catalytic properties, exceeding the state-of-the-art commercial 20% Pt/C catalyst with more positive half-wave potential (15 mV difference, at 1600 rpm), better stability (no significant degradation for UiO-66-NO2@CoCNT vs 19% degradation for 20% Pt/C after 25 000 s), and higher methanol tolerance. When assembled in a flexible zinc–air battery, the UiO-66-NO2@CoCNT remains a competitive alternative to commercial 20% Pt/C catalyst with comparable power density and excellent flexibility, suggesting its potential in wearable electronic devices. The outstanding performance of UiO-66-NO2@CoCNT composite is closely related to the synergetic effect among the three components: CNT as a conductive backbone, cobalt phthalocyanines as the oxygen reduction catalytic active site, and UiO-66-NO2 as an ideal oxygen adsorption pump (the oxygen diffusion rate is 4.8 times that of 20% Pt/C and 17.7 times that of CoCNT). The synergy between the three components facilitates oxygen adsorption, transfer of adsorbed oxygen molecules, oxygen reduction, and electron conduction.
研究领域:
材料科学
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电化学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 13
·5949-5957
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IF 3.591
Xuexia Liu,Shuaihui Li,Limin Liu,Zhijun Wang
The development of active and stable carbon nanomaterials as electrocatalysts for the oxygen reduction reaction (ORR) remains a significant challenge. Herein, we report a one-step pyrolysis process to design hierarchical micro/mesoporous N-doped carbon (m-NC) materials using low-cost folic acid precursors. The optimal m-NC material carbonized at 750 °C (m-NC-750) displays a splendid ORR electrocatalytic activity and perfect stability in an alkaline medium (0.1 mol L−1 KOH). Notably, the current density of m-NC-750 can reach 4.35 mA cm−2 at 0.85 V, which surpasses that of commercial Pt/C (20 wt%). The higher electrocatalytic activity and activation of oxygen is due to the porous structures facilitating ion diffusion and the graphitic N dopant providing more active sites. In addition, the graphite N dopant of the m-NC material possesses the lowest energy barrier of reactions based on density functional theory (DFT) calculations, which effectively boosts the ORR of the as-prepared materials. This simple and economical method provides a facile way of designing high-performance carbon electrocatalysts for the ORR.
研究领域:
材料科学
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电化学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2016
·Vol. 163
·期 9
·H738
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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
ChemCatChem
·
2022
·Vol. 14
·期 10
·e202200063
·
IF 5.497
Liyan Wang,Sheng-Qi Guo,Zhenzhong Hu,Boxiong Shen,Wei Zhou
Graphical Biomass waste-derived electrocatalyst : A biomass waste-derived N-doped honeycomb-like carbon electrocatalyst by one-step pyrolysis. g-C 3 N 4 is used as a multifunctional template to control the morphology of the catalyst and provide a source of N. The catalyst delivers remarkable ORR activity and zinc-air battery performance with fast discharge and higher current density. Exploring an effective way to convert biomass waste into highly active oxygen reduction reaction (ORR) electrocatalysts will not only benefit alleviating environmental management pressure, but also open up new ways for the development of alternatives to Pt-based catalysts. Although the traditional pyrolysis conversion method has been proved to be stable and feasible, the low electrocatalytic activity of the product and the cumbersome post-treatment process make it difficult to be popularized. Here, we report an effective method to overcome the mentioned drawbacks: the introduction of g-C 3 N 4 . The experimental results confirm that g-C 3 N 4 can be used as a multifunctional template for adjusting the morphology and providing N source. More importantly, it will decompose at 700 °C and avoid post-treatment of residues. The pyrolysis products assisted by g-C 3 N 4 exhibit similar ORR performances to commercial Pt/C, including onset potential of 0.963 V (vs. RHE), half-wave potential of 0.835 V (vs. RHE) and limiting current density of 6.35 mA ⋅ cm −2 . Impressively, the product displayed outstanding performance on output power density (107 mW ⋅ cm −2 ) and discharge performance at different current densities as the air electrode of zinc-air battery, which even superior to that of commercial Pt/C. This study elucidated the functional role of g-C 3 N 4 in reaction system and facilitated the development of more efficient biomass waste-based ORR electrocatalysts.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2017
·
IF 6.395
Tao Fu,Jianxing Huang,Shaobo Lai,Size Zhang,Jun Fang,Jinbao Zhao
The catalytic activity and stability of electrocatalyst is critical for the commercialization of fuel cells, and recent reports reveal the great potential of the hollow structures with Pt skin coat for developing high-powered electrocatalysts due to their highly efficient utilization of the Pt atoms. Here, we provide a novel strategy to prepare the Pt skin coated hollow Ag-Pt structure (Ag-Pt@Pt) of ∼8 nm size at room temperature . As loaded on the graphene, the Ag-Pt@Pt exhibits a remarkable mass activity of 0.864 A/mg Pt (at 0.9 V, vs. reversible hydrogen electrode (RHE)) towards oxygen reduction reaction (ORR), which is 5.30 times of the commercial Pt/C catalyst, and the Ag-Pt@Pt also shows a better stability during the ORR catalytic process. The mechanism of this significant enhancement can be attributed to the higher Pt utilization and the unique Pt on Ag-Pt surface structure, which is confirmed by the density functional theory (DFT) calculations and other characterization methods. In conclusion, this original work offers a low-cost and environment-friendly method to prepare a high active electrocatalyst with cheaper price, and this work also discloses the correlation between surface structures and ORR catalytic activity for the hollow structures with Pt skin coat, which can be instructive for designing novel advanced 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
Journal of Materials Chemistry A
·
2014
·Vol. 2
·期 34
·14071-14081
·
IF 0
Zhong-Jie Jiang,Zhongqing Jiang
Nitrogen-doped hollow graphene microspheres (NHGSs), synthesized through a procedure involving the calcination of graphene–oxide-wrapped amine-functionalized mesoporous silica nanoparticles (AFMSNs) and the subsequent removal of the AFMSNs via HF etching, have been employed as an electrocatalyst for the oxygen reduction reaction (ORR). It has been shown that these NHGSs are highly active toward ORR and exhibit higher electrocatalytic activity than graphene, nitrogen-doped graphene (NG), hollow graphene microspheres (HGSs), and JM Pt/C 40 wt%, and a comparable overpotential to JM Pt/C 40 wt%. Their high electrocatalytic activity could be attributed to the N-doped graphitic structure, which produces more active sites for the ORR, allowing the easier adsorption of oxygen and the subsequent reduction; and the specific microspherical hollow structure, which promotes the exposure of more surface area accessible to electrolytes, thereby allowing an easier diffusion of electrolytes into and out of the electrode catalyst layers. Their low overpotential for the ORR can be attributed to the specific microspherical hollow structure, which reduces the overpotential contribution from the mass transport limitation. The stability measurements show that NHGSs also exhibit a much higher stability than graphene, NG, HGSs, and JM Pt/C 40 wt%, and are immune to the methanol crossover and CO poisoning effects, which all together makes NHGSs highly attractive as an electrocatalyst for the ORR.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
CARBON
·
2014
·
IF 6.16
Rui Ning,Chenjiao Ge,Qian Liu,Jingqi Tian,Abdullah M. Asiri,Khalid A. Alamry,Chang Ming Li,Xuping Sun
Hierarchically porous N-doped carbon nanoflakes (HPNCNFs) were facilely synthesized on a large scale via pyrolysis of 1,8-diaminonaphthalene (DAN)/FeCl 3 ·6H 2 O mixture under Ar followed by acid leaching. Both pyrolysis temperature and the amount of Fe species have strong influence on catalyst activity. It suggests that the presence of large excess Fe species not only is key to nanoflake formation but also serves as a mesopore-forming agent. The HPNCNF-900 catalyst, obtained at 900 °C with a mass ratio 1:5 of DAN to FeCl 3 ·6H 2 O, was found to exhibit superhigh oxygen reduction reaction activity and excellent durability in alkaline media outperforming the state-of-the-art Pt/C catalyst at a moderate loading.
研究领域:
材料科学
·
电化学
✓ 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）