INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Lei Liu,Huan Liu,Xingwei Sun,Chunping Li,Jie Bai
Transition metal iron-based catalysts are promising electrocatalysts for oxygen reduction reaction (ORR), and they have the potential to replace noble metal catalysts . The one-dimensional of carbon nanofibers with tubular structure can effectively promote the electrocatalytic activity , which facilitates electron transport . Herein, the Pt–Fe/CNFs were synthesized by electrospinning and subsequent calcination . Benefiting from the advantages of one-dimensional structure, Pt–Fe/CNFs-900 with fast electrochemical kinetics and excellent stability for ORR with excellent onset of 0.99 V, a low Tafel slope of 62 mV dec −1 and high limiting current density of 6.00 mA cm −2 . Long-term ORR testing indicated that the durability of this catalyst was superior to that of commercial Pt/C in alkaline electrolyte . According to RRDE test, the ORR reaction process of Pt–Fe/CNFs-900 was close to four-electron transfer routes.
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Science Bulletin
·
2019
·
IF 6.277
Junbo Zhang,Xiaolin Li,Ming Xu,Yusen Yang,Yinwen Li,Ning Liu,Xiaoyu Meng,Lifang Chen,Shuxian Shi,Min Wei
Glycerol (GLY) aerobic oxidation in an aqueous solution is one of the most prospective pathways in biomass transformation, where the supported catalysts based on noble metals (mainly Au, Pd, Pt) are most commonly employed. Herein, Pt nanoparticles supported on rehydrated Mg x Al 1 -hydrotalcite (denoted as re-Mg x Al 1 -LDH-Pt) were prepared via impregnation-reduction method followed by an in situ rehydration process, which showed high activity and selectivity towards GLY oxidation to produce glyceric acid (GLYA) at room temperature. The metal-support interfacial structure and catalyst basicity were modulated by changing the Mg/Al molar ratio of the hydrotalcite precursor, and the optimal performance was achieved on re-Mg 6 Al 1 -LDH-Pt with a GLY conversion of 87.6% and a GLYA yield of 58.6%, which exceeded the traditional activated carbon and oxide supports. A combinative study on structural characterizations (XANES, CO-FTIR spectra, and benzoic acid titration) proves that a higher Mg/Al molar ratio promotes the formation of positively charged Pt δ + species at metal-support interface, which accelerates bond cleavage of α-C–H and improves catalytic activity. Moreover, a higher Mg/Al molar ratio provides a stronger basicity of support that contributes to the oxidation of terminal-hydroxyl and thus enhances the selectivity of GLYA. This catalyst with tunable metal-support interaction shows prospective applications toward transformation of biomass-based polyols.
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高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 23
·7151-7160
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IF 6.177
Yaxin Zhou,Hao Qin,Sihan Fang,Yangyang Wang,Jun Li,Giuseppe Mele,Chen Wang
Photocatalytic hydrogen production from water is a clean and sustainable way of energy regeneration. Single-atom catalysts (SACs) have received increasing attention in the field of photocatalysis due to their high catalytic activity, selectivity, stability, and 100% atomic utilization. In this work, we utilized TiO2 with oxygen vacancy (Vo-TiO2) to anchor atomically dispersed Pt and Pd, developing a Vo-TiO2-supported dual atomic catalyst (Pt–Pd SAs/Vo-TiO2). Experiments show the metal atomic sites are stabilized by the oxygen vacancy of TiO2, and the Ti–Pt–Ti structure and the Ti–Pd–Ti structure are constructed. The result shows that the hydrogen production rate of Pt–Pd SAs/Vo-TiO2 is 4 times higher than that of Pt–Pd NPs/TiO2, and its hydrogen production rate is as high as 4241.4 μmol h−1 gcat.−1, which greatly reduces catalyst cost and makes photocatalytic water hydrogen production more economical and sustainable. This work provides a new idea for the development of dual single-atom catalysts for efficient photocatalytic hydrogen production.
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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Binbin Zhao,Jieqi Zou,Chen Chen,Qian He,Qiong Tang,Lei Liu,Jinxiang Dong
Pt-WO x -based catalyst has been considered as a promising candidate for the conversion of glycerol to 1,3-propanediol, but the catalytic performance was quite susceptible to the structure and chemical state of WO x species. Herein, we develop a facile approach to construct the single-atom tungsten-doped Al 2 O 3 with a low chemical state through in-situ migration of WO 3 nanoparticles under the H 2 atmosphere. The characterization results demonstrated that the tetrahedral W 5+ could disperse and stabilize the platinum species more effectively, and exhibited stronger interaction with platinum than the octahedral W 6+ species. The enhanced catalytic performance is attributed to the rich oxygen defects on in-situ generated tetrahedral WO x on the catalyst, which facilitated the construction of Pt-WO x interface and strengthened the synergetic effects between them. The analysis of structure-performance correlation revealed that the mono-dispersed tetrahedral W 5+ species [(-O-) 3 W(=O)] played a pivotal role in tuning catalyst acidity and improving the catalytic performance, which assists the adsorption of glycerol and captures H for in-situ formation of Brønsted acid site, and ultimately affected the selectivity toward 1,3-PDO and catalytic activity.
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Materials Today Chemistry
·
2023
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IF 7.3
Xiaodong Zhang,Renzhi Rao,Bin Gao,Shuting Ma,Fukun Bi,Chenyu Li,Ziqiao Zhu,Ning Liu,Yiqiong Yang,Zhong Wang
The crystal engineering of metal oxide supports aims to enhance the performance of precious metal catalysts in semi-volatile organic compounds (SVOCs). Di (2-ethylhexyl) phthalate (DEHP) as one of the representative SVOCs in indoor environments, has become a research hotspot in recent years. For the catalytic oxidation of DEHP, Pt/TiO 2 catalysts were prepared on supports of TiO 2 with different crystalline phases (mixed phase (P25), anatase, and rutile). P25 exhibits a higher PtO x content due to its unique mixed crystalline phase, giving the best catalytic performance of the synthesized catalyst through light, thermal and photothermal catalytic experiments. The degradation of DEHP is optimized by a combination of photocatalysis and thermal catalysis. The intermediates and degradation pathways were analyzed through GC-MS and other characterization methods, and the possible degradation pathways were schematically studied. This work provides the possibility to rationalize the design of photothermal catalysts for SVOC removal.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Xianrong Liu,Kunjie Wang,Yongcheng Li,Yunsi Wang,Bingxin Liu,Peng Zhang,Benhua Xu
Platinum (Pt) is the state-of-the-art electrochemical catalyst for hydrogen evolution reaction (HER), but its commercial developments are restricted by scarcity and high cost. In this paper, defective porous carbon is obtained by removing the doped nitrogen atoms at high temperatures and ultrafine Pt nanoparticles were embedded in the defective porous carbon (Pt NPs/DPC) via a facile hydrothermal method . Benefiting from the synergistic effect of ultrafine Pt NPs and conductive substrate, Pt NPs/DPC catalyst exhibits high electrochemical activity with a low overpotential of 30 mV at 10 mA cm −2 and Tafel slope of 31 mV dec −1 and remarkable long-term electrochemical stability in acid solution, demonstrating HER performance superior to commercial 40 % Pt/C.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2023
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IF 4.5
Shixin Zhang,Huanqiao Song,Tianjiao Li,Mingsheng Luo,Yu Chen,Changke Shao
Developing catalysts for the stable electrooxidation of ethanol have been a goal pursued by scientists. The present work reports a facile synthesis of catalysts with a double junction structure of Pt and SnO 2 on graphene (Pt/SnO 2 GN) through sol–gel combined with glycol hydrothermal reduction method. The physicochemical analyses show that the reduced Pt uniformly dispersed on GN is located adjacent to SnO 2 and has electronic interaction with the composite carrier. The electrochemical results exhibit that Pt/SnO 2 GN has better catalytic performance for ethanol electrooxidation than PtSnO 2 /GN and PtSn/GN. The ethanol oxidation peak current density on Pt/SnO 2 GN, after 1500 cycles of voltammetric testing, can still maintain 99.2% of the highest. The excellent catalytic stability of Pt/SnO 2 GN is ascribed to the double junction structure and the appropriate interaction between Pt and SnO 2 on GN, which enlarge the ECSA of Pt, improve the structural integrity, accelerate the charge transfer kinetics and increase the CO tolerance.
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Carbon Letters
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2023
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IF 4.5
Yang Yang,Hu Huali,Ai Jixing,Wang Hong,Du Haijun
Sulfamonomethoxine (SMM) is widely used to inhibit Gram-positive and Gram-negative bacteria, and improper use of SMM is detrimental to human health and ecological stability. Therefore, a sensitive determination method is of great importance for monitoring SMM residues in water, meat, milk, eggs, etc. Herein, a Pt-functionalized S-doped graphitic carbon nitride (Pt/S-g-C 3 N 4 ) was constructed for the electrochemical determination of SMM. The as-developed Pt 3 /S 3 -g-C 3 N 4 sensor showed a significant SMM determination performance. The electrochemical oxidation of SMM on Pt 3 /S 3 -g-C 3 N 4 /GCE involves two electron transference and was limited by a diffusion process. The as-developed Pt 3 /S 3 -g-C 3 N 4 /GCE sensor has good linearity in a wide range of 0.1–120 μmol/L and a remarkably low limit of detection (LOD) of 0.026 μmol/L for SMM determination. In addition, the sensor has high selectivity and anti-interference properties for SMM detection. Furthermore, this Pt 3 /S 3 -g-C 3 N 4 /GCE sensor has good reproducibility and stability. Moreover, the recoveries were in the range of 89.6–112.2% for the detection of the SMM in a real sample of egg. The proposed Pt 3 /S 3 -g-C 3 N 4 /GCE sensor shows great potential for practical applications in detecting trace amounts of antibiotics.
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Surfaces and Interfaces
·
2023
·
IF 6.2
Caiqin Wang,Tingting Zhou,Cheng Qian,Lili Chen,Liyuan Hao,Shumeng Fu,Bingguo Feng,Xiaofei Yang
Ti 3 C 2 T x MXene nanonets (MNNs) with 3D fibrous architecture were obtained from Ti 3 C 2 T x MXene nanoplates (MNPs) via surface modifying of alkalization in concentrated KOH solution, which was further combined with carbon nanotube and used as catalyst supports for Pt nanoparticles. By controlling the treatment time of alkalization, the lamellar surface of MNPs was getting into fibration in different extent. The catalytic performances toward hydrogen evolution reaction (HER) of a series of Pt-loaded MNNs catalysts were investigated, in which 1 %Pt-MNNs-9 composite catalyst presented the best hydrogen evolution performance. In detail, 1 %Pt-MNNs-9 with 1 wt.% of Pt loading exhibits an overpotential of 60 mV at 10 mA·cm −2 , which is much lower than 1 % Pt-MNPs (274 mV). It also keeps stable performance for long term stability. The enhanced catalytic activity is probably due to the fact that, Ti 3 C 2 T x MNNs with 3D architecture not only possesses abundant sites to anchor Pt nanoaprticles, but also facilitates the mass and charge transfer, which are significantly beneficial to catalytic reaction. The 3D architecture MXene fibers are expected to have widespread applications including but not limited to energy storage/conversion, and catalytic fields.
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ChemistrySelect
·
2023
·Vol. 8
·期 37
·e202301117
·
IF 2.1
Mengting Chen,Meihua Zhang,Xiaoshuang Liu,Yingxin Liu
Graphical Herein, we report a highly efficient synthesis of N -arylhydroxylamines through controllable hydrogenation of nitroarenes using hydrazine hydrate as a hydrogen donor over Pt/C catalyst at a low temperature (30 °C). The synthesis of N -arylhydroxylamines through the in-situ hydrogenation of nitroarenes over commercial Pt/C catalyst was investigated. The effects of various reaction conditions including hydrogen donor, solvent, catalyst dosage, temperature and reaction time on the selective hydrogenation of nitrobenzene (NB) to N -phenylhydroxylamine (PHA) were systematically investigated. The results showed that the yield of N -phenylhydroxylamine reached 87.2 % using hydrazine hydrate as hydrogen donor in N,N -dimethylformamide solvent at 30 °C for 60 min. And the catalyst showed no obvious activity loss after a 6-times recycle. Meanwhile, the developed methodology can also transform a range of nitroarenes to the corresponding N -arylhydroxylamines in excellent yields (74–99 %).
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Catalysts
·
2021
·Vol. 11
·期 4
·478
·
IF 4.146
Zhen Song,Jiameng Wang,Fanji Liu,Xiqing Zhang,Énio Matusse,Lihong Zhang
Here, a simple method was developed to prepare an MgF2-modified hydrotalcite-derived composite, which was used as support for the Pt-In catalyst for isobutane direct dehydrogenation. The catalysts, composites, and their precursors were characterized by numerous characterization techniques. The results provided evidence for the MgF2promoter effect on the physical–chemical properties and dehydrogenation performance of the supported Pt-In catalysts. The catalyst with MgF2shows exceptional isobutene selectivity that can be stabilized at 95%, and the conversion increases from 50% to 58% during the reaction process. Moreover, the existence of MgF2plays an important role in the resistance to coke formation and Pt sintering by improving the Pt dispersion, inhibiting the reduction of the In3+species, and adjusting the acidity of the catalyst.Keywords:isobutane dehydrogenation;MgF2promoter;hydrotalcite-derived composites;supported Pt-In catalysts
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Zexiang Lv,Shanhui Zhu,Sen Wang,Mei Dong,Zhangfeng Qin,Jianguo Wang,Weibin Fan
A series of CoAl oxide-supported Pt catalysts (Pt/CoxAl, x = Co/Al ratio) was developed for aqueous-phase reforming of methanol to H 2 . CoxAl oxides were prepared by calcining layered double hydroxides at different temperatures. The catalytic performance of Pt/CoxAl highly depends on the Co/Al ratio and the calcination temperature. The most active Pt/Co2Al catalyst calcined at 700 °C showed an H 2 production rate of 3372 µmol H2 ·g −1 catalyst ·min −1 with low CO selectivity. The intense interaction between Pt and support and abundant oxygen vacancies results in high catalytic performance. Intensive characterization and mechanism study reveal that both Pt 0 and metallic Co 0 promote methanol decomposition. At the same time, H 2 O is activated on the support and reacts with CO to generate intermediate formate species that are further converted into CO 2 and H 2 .
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