Carbon Energy
·
2023
·Vol. 5
·期 9
·e339
·
IF 20.5
Chenjie Han,Yeqing Lyu,Shaona Wang,Biao Liu,Yi Zhang,Jun Lu,Hao Du
Due to their environmentally friendly nature and high energy density, direct ethanol fuel cells have attracted extensive research attention in recent decades. However, the actual Faraday efficiency of the ethanol oxidation reaction (EOR) is much lower than its theoretical value and the reaction kinetics of the EOR is sluggish due to insufficient active sites on the electrocatalyst surface. Pt/C is recognized as one of the most promising electrocatalysts for the EOR. Thus, the microscopic interfacial reaction mechanisms of the EOR on Pt/C were systematically studied in this work. In metal hydroxide solutions, hydrated alkali cations were found to bind with OH ad through noncovalent interactions to form clusters and occupy the active sites on the Pt/C electrocatalyst surface, thus resulting in low Faraday efficiency and sluggish kinetics of the EOR. To reduce the negative effect of the noncovalent interactions on the EOR, a shield was made on the electrocatalyst surface using 4-trifluoromethylphenyl, resulting in twice the EOR catalytic reactivity of Pt/C.
研究领域:
电化学
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催化
·
材料科学
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能源材料
✓ 已验证
产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2024
·
IF 3.5
Yang Mingzhu,Li Liangli,Shi Jingjing,Xia Haian,Xu Junming
Lignin is an important source of biomass energy and chemical raw material. The combination of lignin depolymerization and electrocatalytic hydrogenation (ECH) is a very important pathway to convert lignin to high-value chemicals or bio-fuels, which has important economic and environmental significance. It remains great challenges to control the conversion pathways and modulate the desired product selectivity. In additions, in-depth understanding of the hydrodeoxygenation mechanism of lignin pyrolysis oil in ECH has not yet been revealed. Herein, we report the results of ECH of various typical lignin models using Pt/C in a fluid electrocatalytic system. Common phenolic model compounds with different functional groups and varying chain lengths were chosen as the reaction substrates, such as guaiacol, 2,6-dimethoxyphenol, eugenol, phenol, vanillin. The effects of the types and positions of functional groups such as hydroxyl, methoxyl and alkyl groups on the ECH performances were investigated. The electrolytic hydrogenation system employed phosphotungstic acid (PW12) and phosphoric acid as the electrolyte, NaBH 4 as a partial hydrogen source and PW12 reducing agent, and Pt/C as the catalyst directly added to the electrolyte. Results demonstrated that the production of cyclohexane from the ECH of the phenolic model compounds, which have undergone complete deoxygenation. For phenolic compounds containing alkyl substituents, the conversion decreases with increasing chain length, but the selectivity of alkyl cyclohexane increases. These findings contribute to advancing the understanding of lignin utilization and pave the way for sustainable development and energy transformation.
研究领域:
生物质化学
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催化化学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 5
·571
·
IF 4.501
Yuxin Liu,Jing Ye,Fanpeng Kong,Chunyu Du,Pengjian Zuo,Lei Du,Geping Yin
Proton exchange membrane (PEM) fuel cells using Pt-based materials as electrocatalysts have achieved a decent performance, represented by the launched Toyota Mirai vehicle. The ideal PEM fuel cells consume stored pure hydrogen and air. However, SO2, as a primary air contaminant, may be fed along with air at the cathode, leading to Pt site deactivation. Therefore, it is important to improve the SO2tolerance of catalysts for the stability of the oxygen reduction reaction (ORR). In this work, we develop the Pt/C-TiO2catalyst against SO2poisoning during ORR. Impressively, the hybrid Pt/C-TiO2catalyst with 20 mass % TiO2shows the best ORR and anti-toxic performance: the kinetic current density of ORR is 20.5% higher and the degradation rate after poisoning is 50% lower than Pt/C. The interaction between Pt and TiO2as well as the abundant hydroxyl groups on the surface of TiO2are both revealed to account for the accelerated removal of poisonous SO2on Pt surfaces.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2017
·
IF 3.091
Qiurong Tian,Zihao Zhang,Feng Zhou,Kequan Chen,Jie Fu,Xiuyang Lu,Pingkai Ouyang
The role of solvents in the conversion of oleic acid over Pt/C was studied. Three solvent systems (solvent-free, water, and dodecane systems) were employed for the conversion of oleic acid over Pt/C at 350 °C. Decarboxylation, hydrogen transfer, and aromatization were observed in these three reaction systems. In comparison to the non-solvent reaction system, much slower decarboxylation and aromatization rates and fewer heptadecane and aromatic products were observed in the hydrothermal and dodecane reaction systems. The decarboxylation and aromatization rates and yields of heptadecane and aromatics decreased with increased dodecane loading in the dodecane reaction system, and the decarboxylation and aromatization rates and yields of heptadecane and aromatics significantly decreased with the increase of water in the hydrothermal reaction system. The effects of solvent loading, catalyst loading, and reaction time on the reactions (decarboxylation, hydrogen transfer, and aromatization) were investigated. The reaction behaviors of 1-heptadecene with different solvents were studied, and N2 adsorption–desorption and thermogravimetric analysis of fresh and spent Pt/C in the three reaction systems were also performed. The results indicate that the competition of dodecane for the Pt/C active sites is mainly responsible for the slow decarboxylation and aromatization rates. In addition to the similar influencing factor to that in the dodecane system, H+ released from water and hydrogen bonding, which inhibited the ionization of carboxyl groups, was the key influencing factor for the slower decarboxylation and aromatization rates obtained under hydrothermal conditions.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
Chemistry-An Asian Journal
·
2024
·Vol. 19
·期 14
·e202400342
·
IF 3.5
Yuanxin Cao,Xiaoming Yu,Tianfu Wang,Jiahao Li,Nan Li,Anbang Ge,Jie Ying,Tongwen Yu
Here, we report the systematical synthesis of zeolite-templated carbon (ZTC) supported Ru and Rh mono- or bi-metallic electrocatalysts towards hydrogen evolution reaction (HER). The zeolite A or ZSM-5 derived ZTC supports and metal sites were adjusted, and all electrocatalysts outperformed the commercial Pt/C electrocatalyst for HER performance. In particular, the RhRu/(ZTC/ZSM5) sample exhibited superior catalytic performance with the overpotential of 24.8 mV@10 mA ⋅ cm −2 , and outstanding stability with 1 mV drop after 20000 cyclic voltammetry circles. This work offers a simple impregnation method for the synthesis of highly performed HER electrocatalysts supported on porous zeolite-templated carbon.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Sustainable Systems
·
2020
·Vol. 4
·期 7
·2000065
·
IF 4.869
Wenrui Yan,Yan Xiang,Jin Zhang,Shanfu Lu,San Ping Jiang
Development of direct formic acid fuel cell (DFAFC) is significantly constrained by low output performance and poor durability because of the sluggish formic acid oxidation reaction (FAOR) and the poisoning by CO ads intermediate on the Pt-based electrocatalyst at low operating temperatures. By operating DFAFCs at elevated temperatures, the peak power density (PPD) of the cell based on the Pt/C catalyst increases significantly. For example, the PPD of DFAFC reaches 198 mW cm −2 at 240 °C, eight times higher than that of the DFAFC at 70 °C. The study shows the surprising transition in power performance of DFAFCs at elevated temperatures. The increase of PPD for DFAFC against temperature is 121 mW cm −2 /100 °C at temperatures above 115 °C, almost three times higher than the 45 mW cm −2 /100 °C obtained at lower temperatures. The fundamental reason for the substantially enhanced power output and durability is the gradual transformation of the reaction kinetics from sluggish direct FAOR at low temperatures to fast H 2 oxidation reaction at elevated temperatures due to the increased in situ decomposition of formic acid on Pt/C catalysts at temperatures above 100 °C. This study demonstrates that operation at temperatures above 160 °C is most effective to promote performance and durability of DFAFCs.
研究领域:
能源科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Xiaojun Zhao,Lijuan Liu,Weiting Yang,Qinhe Pan
The utilization of hydrogen energy is an effective way to alleviate the shortage of traditional energy, carbon emissions, and environmental pollution. As a hydrogen energy conversion device, fuel cells are severely limited by the slow oxygen reduction reaction on the cathode. Herein, we designed and synthesized the composite precursors of ZIF and chitosan, which was used for the preparation of a series of efficient carbon-based catalysts for oxygen reduction by pyrolysis. Among them, ZnCo-ZIF@CS-3-800 shows the best catalytic performance. Its onset potential and limited current density are nearly the same as those of Pt/C, and its half-wave potential is 9 mV higher than that of Pt/C. Moreover, it also exhibits excellent catalytic stability, durability, and methanol tolerance, promising great potential and prospects for application in fuel cells.
研究领域:
材料科学
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能源科学
·
催化
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 21
·12689-12694
·
IF 3.119
Na Gao,Xingqiao Wu,Xiao Li,Jingbo Huang,Dongsheng Li,Deren Yang,Hui Zhang
Developing an efficient Pt-based multimetallic electrocatalyst with well-defined shapes for methanol oxidation reaction (MOR) is critical, however, it still remains challenging. Here we report a one-pot approach for the synthesis of ternary PtPdCu alloy hexapods with different compositions. Their MOR activities increased in the sequence Pt2PdCu4 < Pt3PdCu4 < Pt5PdCu5, and were substantially higher than that of commercial Pt/C. Specifically, the Pt5PdCu5 hexapods exhibited the highest mass (0.97 mA μgPt−1) and specific (7.39 mA cm−2) activities towards MOR, and were 5.4 and 19.4 times higher than those of commercial Pt/C (0.18 mA μgPt−1 and 0.38 mA cm−2), respectively. This enhancement could be probably attributed to the bifunctional mechanism and ligand effect through the addition of Cu and Pd as well as the unique dendritic structure. The better tolerance for CO poisoning also endowed the PtPdCu hexapods with superior durability relative to commercial Pt/C.
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
FUEL
·
2023
·
IF 7.4
Xiaoying Qi,Na Ye,Riguang Zhang,Zhao Jiang,Tao Fang
Developing the efficient and high CO tolerance electrocatalysts is important for methanol oxidation reaction. In this study, a sequence of catalysts were constructed by introducting various transition metal nitrides (TMNs) to modify the Pt/C catalyst. The corresponding electrochemical performance were evaluated to investigate the activity, kinetics, charge transfer rate, CO tolerance and stability for MOR in alkaline media. Based on the structural characterization analysis from ICP-MS, XRD, HRTEM and XPS, it could be indicated that the participation of TMNs mainly brought the electronic effect, but not for the geometric effect. The evident difference did not exist in the nanoparticle size, morphology and crystallinity of the related catalysts. After the evaluation on the catalytic performance for alkaline MOR, The TMNs-modified catalysts exhibited higher activity and lower onset potential potential compared with the commercial Pt/C. Among them, Pt-NbN/C showed the highest mass activity with 9.56-fold that of the commercial Pt/C. The faster charge transfer kinetics and reaction rate were confirmed by Tafel and EIS results. CA measurements indicated that they also exhibited higher stability and anti-CO poisoning ability for alkaline MOR, consistent with the CO stripping experiments. To quantitatively describe the realtionship of the electronic effect on the catalytic activity and CO tolerance, the d-band center was employed as a parameter to bulid the corresponding function. Interestingly, it was proposed that the rational d-band center could lead high MOR performance and anti-CO poisoning ability. The introduction of TMNs brought the evident shift of the Pt d-band center and boosted the catalytic activity and anti-CO poisoning ability for alkaline MOR.
研究领域:
电化学
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2026
·
IF 4.1
Yunlin Bai,Tianhe Li,Hao Chen,Yang Xu,Jiahao Ji,Guanghua Wei,Junfang Cheng
Developing efficient and durable oxygen reduction reaction (ORR) catalysts is critical for advancing proton exchange membrane fuel cells (PEMFCs). While Pt-based alloy catalysts exhibit enhanced ORR activity, their disordered nanostructures often compromise durability. In this work, a carbon-supported Pt 3 Cu alloy catalyst with a core-shell architecture (Pt 3 Cu@Pt/C) was synthesized via a controlled impregnation-reduction method followed by acid-washing to construct a Pt-rich shell. Comprehensive physicochemical characterizations confirmed the formation of a face-centered cubic (FCC) structure with a Pt 3 Cu core and a Pt-rich shell. Alloying with Cu was found to downshift the Pt d-band center, thereby optimizing the adsorption strength of oxygen intermediates. Electrochemical evaluations revealed that the Pt 3 Cu@Pt/C catalyst exhibited a mass activity (MA) of 0.37 A mg −1 and an electrochemical surface area (ECSA) of 89.43 m 2 g −1 , surpassing commercial Pt/C. Although the core-shell treatment slightly reduced ORR activity compared to untreated Pt 3 Cu/C, the Pt 3 Cu@Pt/C catalyst demonstrated exceptional durability, retaining >70% of its initial ECSA and showing only a 27% decay in MA after 30,000 accelerated stress test cycles, far outperforming both Pt 3 Cu/C and commercial Pt/C. Density functional theory (DFT) calculations revealed that the Pt shell increased Cu vacancy formation energy by 0.8 eV, effectively suppressing Cu dissolution and enhancing structural stability. This work highlights the synergistic electronic and geometric effects of core-shell nanostructures in balancing ORR activity and durability, providing insights for designing advanced Pt-based catalysts.
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xiaoyang Wang,Ziqi Fu,Ziyi Luo,Weidi Liu,Jia Ding,Jianrong Zeng,Yanan Chen,Wenbin Hu
High-loading Pt/C catalysts play an important role in the fabrication of membrane electrode assemblies with thin catalytic layer, which enhance mass transport and maintain the balance of water and heat. Unfortunately, as the loading increases, the agglomeration and growth of Pt nanoparticles (NPs) occur, causing unsatisfactory performance. Here, we present an efficient method for preparing of highly dispersed and small-sized Pt/C catalysts with Pt loadings varying from 39.01 wt% to 66.48 wt% through the high-temperature shock technique. The high density and ultrafine (~2.5 nm) Pt NPs are successfully anchored onto Vulcan XC-72R carbon black without the use of additional capping agents or surfactants. The modified carbon supports enhance the affinity for Pt precursors, contributing to loading efficiencies of 95% or more, while also providing abundant sites for the nucleation and fixation of Pt NPs, thus preventing agglomeration. In the context of the hydrogen evolution reaction in acidic media, the as-synthesized high-loading Pt/C catalysts show remarkable activity and stability, outperforming the state-of-the-art commercial Pt/C. This is mainly because the combined effects of ultrasmall and uniform Pt NPs, optimized electronic structure of Pt site, superhydrophilicity and effective anchoring of Pt NPs. The polymer electrolyte membrane electrolyzer integrated with Pt60/OX72R and commercial IrO 2 reaches 1 A cm –2 at 1.77 V and operates stably for 120 hours with a negligible voltage decay. This new strategy is fast, scalable and cost-effective for large-scale production of metal-supported catalysts, especially for the high-loading ones.
研究领域:
催化化学
·
纳米技术
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材料科学
·
电化学
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chaoqi Han,Wenwen Shi,Mengxue Huang,Qi Wang,Jie Yang,Jingchao Chen,Ruimin Ding,Xi Yin
Understanding the complex solvent effects on the microstructures of ink and catalyst layer (CL) is crucial for the development of high-performance anion exchange membrane fuel cells (AEMFCs). Herein, we study the solvent effects within the binary solvent ink system composed of water, isopropyl alcohol (IPA), commercial anion exchange ionomer, and Pt/C catalyst. The results show that the Pt/C particles and ionomer tend to form large aggregates wrapped with a thick ionomer layer in IPA-rich ink and promote the formation of large mesopores within the CL. With the increase of the water content in the ink, Pt/C particles are more likely to bridge to each other through wrapped FAA to form a well-connected three-dimensional network. The CL fabricated using water-rich ink shows smaller pores, higher porosity, and a more homogeneous ionomer network without the formation of large aggregates. Based on these results, we propose that the properties of the solvent mixture, including dielectric constant (ε) and solubility parameter (δ), affect the coulomb interaction of charged particles and surface tension at interfaces, which in turn affects the microstructure of ink and CL. By leveraging the solvent effects, we optimize the CL microstructures and improve the performance of AEMFC. These results may guide the rational design and fabrication of AEMFCs.
研究领域:
能源科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）