Pt/C catalysts were prepared using black carbon (CB), and evaluated for their potential application as a catalyst of liquid-phase catalystic exchange for tritium treatment. CB was treated with 10% H2O2 solution for 0 and 2 hours at 105°C, Ethylene glycol and 40wt% Pt were added to the dried treated sample to prepare a Pt/C catalyst. The physical and chemical properties of the prepared catalysts were evaluated by BET, XRD, elemental analysis (EA), and TEM analyses. As a result of BET analysis, the surface area of CB without 10% H2O2 was 237.2 m2·g-1, and after treatment with 10% H2O2, it decreased to 181.2 m2·g-1 for 2 hours. However, the internal surface area increased, indicating the possibility that more Pt could be distributed inside the CB treated with 10% H2O2. In the XRD analysis results, the presence of Pt was confirmed by observing the Pt peak in the prepared Pt/C catalyst, and it was also observed through TEM analysis that Pt was evenly distributed within the CB. The elemental analysis (EA) results showed that the ratio of S and N decreased and the ratio of O increased with increasing 10% H2O2 treatment time. The H2O2 treated carbon supported Pt catalysts and polytetrafluoroethylene were then loaded together on a foamed nickel carrier to obtain hydrophobic catalysts. Our hydrophobic Pt catalyst using H2O2 treated black carbon are expected to be usefully used in the tritium treatment system.

Mass production of high-quality carbon nanotubes (CNTs) remains a challenge, requiring the development of new wetimpregnated catalyst suitable for the catalytic chemical vapor deposition (CCVD) of CNTs in a fluidized bed reactor. For the successful development of a new catalyst, a highly robust system to synthesize CNTs must be established. Here, we systematically investigated the robustness of CNT synthesis by CCVD using a wet-impregnated catalyst. We statistically tested four factors that could potentially affect the robustness of CNT synthesis system, focusing on carbon yield and IG/ID. First, we tested the effect of vacuum baking before CNT growth. F test and CV equality test concluded that vacuum baking recipe did not significantly reduce the variability of the CNT synthesis. Second, we tested the batch-to-batch variation of catalysts. The results of t test and one-way analysis of variance indicate that there is significant difference in carbon yield and IG/ID among catalysts from different batches. Third, we confirmed that there is spatial non-uniformity of wet-impregnated catalysts within a batch when they are produced in large scale. Finally, we developed a multi-step heating recipe to mitigate the temperature overshooting during the CNT synthesis. The multi-step recipe increased the mean of carbon yield, but did not influence the variability of CNT synthesis. We believe that our research can contribute to the establishment of a robust CNT synthesis system and development of new wet-impregnated catalysts.

To investigate the effect of the catalyst and metal–support interaction on the methane decomposition behavior and physical properties of the produced carbon, catalytic decomposition of methane (CDM) was studied using Ni/SiO2 catalysts with different metal–support interactions (synthesized based on the presence or absence of urea). During catalyst synthesis, the addition of urea led to uniform and stable precipitation of the Ni metal precursor on the SiO2 support to produce Ni-phyllosilicates that enhanced the metal–support interaction. The resulting catalyst upon reduction showed the formation of uniform Ni0 particles (< 10 nm) that were smaller than those of a catalyst prepared using a conventional impregnation method (~ 80 nm). The growth mechanisms of methane-decomposition-derived carbon nanotubes was base growth or tip growth according to the metal–support interaction of the catalysts synthesized with and without urea, respectively. As a result, the catalyst with Ni-phyllosilicates resulting from the addition of urea induced highly dispersed and strongly interacting Ni0 active sites and produced carbon nanotubes with a small and uniform diameter via the base-growth mechanism. Considering the results, such a Ni-phyllosilicate-based catalyst are expected to be suitable for industrial base grown carbon nanotube production and application since as-synthesized carbon nanotubes can be easily harvested and the catalyst can be regenerated without being consumed during carbon nanotube extraction process.

Electrochemical reduction of carbon dioxide to valuable chemicals is a promising way of storing renewable energy through electric-to-chemical energy conversion, while its large-scale application is in urgent need of cheap and high-performance catalysts. Herein, we invent a convenient method to synthesize N-doped porous carbon by ammonia etching the pyrolysis carbon of petroleum pitch. We found the ammonia etching treatment not only increase the pyridinic-N content, but also enlarge the specific surface area of the petroleum pitch-based porous carbon. As a cheap and easily available catalyst for carbon dioxide electroreduction, up to 82% of Faradaic efficiency towards carbon monoxide was obtained at − 0.9 V vs the reversible hydrogen electrode in 0.1 M KHCO3. After a long time electrocatalysis of more than 20 h, the Faradaic efficiency of carbon monoxide remains 80%, indicating the porous carbon as made have an ultra-high stability as catalyst for carbon dioxide reduction. Our work provides a new technology to economically prepare efficient electrocatalysts for carbon dioxide reduction.

Carbon-encapsulated Ni catalysts are synthesized by an electrical explosion of wires (EEW) method and applied for CO2 methanation. We find that the presence of carbon shell on Ni nanoparticles as catalyst can positively affect CO2 methanation reaction. Ni@5C that is produced under 5% CH4 partial pressure in Ar gas has highest conversions of 68 % at 350 oC and 70% at 400 oC, which are 73 and 75% of the thermodynamic equilibrium conversion, respectively. The catalyst of Ni@10C with thicker carbon layer shows much reduced activity. The EEW-produced Ni catalysts with low specific surface area outperform Ni catalysts with high surface area synthesized by solution-based precipitation methods. Our finding in this study shows the possibility of utilizing carbon-encapsulated metal catalysts for heterogeneous catalysis reaction including CO2 methanation. Furthermore, EEW, which is a highly promising method for massive production of metal nanoparticles, can be applied for various catalysis system, requiring scaled-up synthesis of catalysts.

Carbon materials with tailorable structures and superior properties have great potential applications in environmental protection, energy conversion, and catalysis. Plant biomass as abundant and green non-toxic raw materials has been considered as good precursors for synthesizing heteroatom-doped carbon materials. However, few studies have been reported on the different natures of carbon materials derived from different parts of the same plant biomass. In this study, we prepared carbon materials from the petioles and blades of apricot leaves by direct pyrolysis without additives. Detailed characterizations indicate that these two carbon materials are similar in element composition and graphitization degree, but differ greatly in surface area and pore volume. These differences can be attributed to the different contents of inorganic salts, vascular bundles, and proteins in petioles and blades. When used as catalysts for the oxidation of ethylbenzene, the petiole-derived carbon shows better catalytic performance than the blades derived carbon due to its high surface area, large average pore size, and doped nitrogen atoms. Furthermore, the carbon catalysts derived from the petioles and blades of poplar leaves and parasol tree leaves show the same difference in catalytic reaction, implying that the above-mentioned conclusion is rather universal, which can provide reference for the synthesis of carbon materials from leaves.

Nitrogen (N)-doped protein-based carbon as platinum (Pt) catalyst supports from tofu for oxygen reduction reactions are synthesized using a carbonization and reduction method. We successfully prepare 5 wt% Pt@N-doped protein-based carbon, 10 wt% Pt@N-doped protein-based carbon, and 20 wt% Pt@N-doped protein-based carbon. The morphology and structure of the samples are characterized by field emission scanning electron microscopy and transmission electron micro scopy, and crystllinities and chemical bonding are identified using X-ray diffraction and X-ray photoelectron spectroscopy. The oxygen reduction reaction are measured using a linear sweep voltammogram and cyclic voltammetry. Among the samples, 10 wt% Pt@N-doped protein-based carbon exhibits exellent electrochemical performance with a high onset potential of 0.62 V, a high E1/2 of 0.55 V, and a low ΔE1/2= 0.32 mV. Specifically, as compared to the commercial Pt/C, the 10 wt% Pt@N-doped proteinbased carbon had a similar oxygen reduction reaction perfomance and improved electrochemical stability.

Activated carbon (AC) was modified by ammonium persulphate or nitric acid, respectively. AC and the modified materials were used as catalyst supports. The oxygen groups were introduced in the supports during the modifications. All the supports were characterized by N2-physisorption, Raman, X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and thermogravimetric analysis. Methanol synthesis catalysts were prepared through wet impregnation of copper nitrate and zinc nitrate on the supports followed by thermal decomposition. These catalysts were measured by the means of N2-physisorption, X-ray diffraction, XPS, temperature programmed reduction and TEM tests. The catalytic performances of the prepared catalysts were compared with a commercial catalyst (CZA) in this work. The results showed that the methanol production rate of AC-CZ (23 mmol- CH3OH/(g-Cu·h)) was higher, on Cu loading basis, than that of CZA (9 mmol-CH3OH/ (g-Cu·h)). We also found that the modification methods produced strong metal-support interactions leading to poor catalytic performance. AC without any modification can prompt the catalytic performance of the resulted catalyst.

To improve the methanol electro-oxidation in direct methanol fuel cells(DMFCs), Pt electrocatalysts embedded on porous carbon nanofibers(CNFs) were synthesized by electrospinning followed by a reduction method. To fabricate the porous CNFs, we prepared three types of porous CNFs using three different amount of a styrene-co acrylonitrile(SAN) polymer: 0.2 wt%, 0.5 wt%, and 1 wt%, respectively. A SAN polymer, which provides vacant spaces in porous CNFs, was decomposed and burn out during the carbonization. The structure and morphology of the samples were examined using field emission scanning electron microscopy and transmission electron microscopy and their surface area were measured using the Brunauer- Emmett-Teller(BET). The crystallinities and chemical compositions of the samples were examined using X-ray diffraction and X-ray photoelectron spectroscopy. The electrochemical properties on the methanol electro oxidation were characterized using cyclic voltammetry and chronoamperometry. Pt electrocatalysts embedded on porous CNFs containing 0.5 wt% SAN polymer exhibited the improved methanol oxidation and electrocatalytic stability compared to Pt/conventional CNFs and commercial Pt/ C(40 wt% Pt on Vulcan carbon, E-TEK).

Nanosized Pt, Pt-Ru and Pt-CeO2 electrocatalysts supported on acid-treated carbon nanotube (CNT) were synthesized by microwave-assisted heating of polyol process using H2Cl6Pt·6H2O, RuCl3, CeCl3 precursors, respectively, and were characterized by XRD and TEM. And then the electrochemical activity of methanol oxidation for catalyst/CNT nanocomposite electrodes was investigated. The microwave assisted polyol process produced the nano-sized crystalline catalysts particles on CNT. The size of Pt supported on CNT was 7~12 nm but it decreased to 3~5 nm in which 10wt% sodium acetate was added as a stabilizer during the polyol process. This fine Pt catalyst particles resulted in a higher current density for Pt/CNT electrode. It was also found that 10 nm size of PtRu alloys were formed by polyol process and the onset potential decreased with Ru addition. Cyclic voltammetry analysis revealed that the Pt75Ru25/CNT electrode had the highest electrochemical activity owing to a higher ratio of the forward to reverse anodic peak current. And the chronoamperemetry test showed that Pt75Ru25 catalyst had a good catalyst stability. The activity of Pt was also found to be improved with the addition of CeO2.

Different oxidation treatments on CNTs using diluted 4.0 M H2SO4 solution at room temperature and or at 90℃ reflux conditions were investigated to elucidate the physical and chemical changes occurring on the treated CNTs, which might have significant effects on their performance as catalyst supports in PEM fuel cells. Raman spectroscopy, X-ray diffraction and transmission electron microscope analyses were made for the acid treated CNTs to determine the particle size and distribution of the CNT-supported Pt-Ru nanoparticles. These CNT-supported Pt-based nanoparticles were then employed as anode catalysts in PEMFC to investigate their catalytic activity and single-cell performance towards H2 oxidation. Based on PEMFC performance results, refluxed Pt-Ru/CNT catalysts prepared using CNTs treated at 90℃ for 0.5 h as anode have shown better catalytic activity and PEMFC polarization performance than those of the commercially available Pt-Ru/C catalyst from ETEK and other Pt-Ru/CNT catalysts developed using raw CNT, thus demonstrating the importance of acid treatment in improving and optimizing the surface properties of catalyst support.

The electrocatalytic characteristics of oxygen reduction reaction of the PtxM(1-x) (M = Co, Cu, Ni) supported on multi-walled carbon nanotubes (MWNTs) have been evaluated in a Polymer Electrolyte Membrane Fuel Cell (PEMFC). The PtxM(1-x)/MWNTs catalysts with a Pt : M atomic ratio of about 3 : 1 were synthesized and applied to the cathode of PEMFC. The crystalline structure and morphology images of the PtxM(1-x) particles were characterized by X-ray diffraction and transmission electron microscopy, respectively. The results showed that the crystalline structure of the Pt alloy particles in Pt/MWNTs and PtxM(1-x)/MWNTs catalysts are seen as FCC, and synthesized PtxM(1-x) crystals have lattice parameters smaller than the pure Pt crystal. According to the electrochemical surface area (ESA) calculated with cyclic voltammetry analysis, Pt0.77Co0.23/MWNTs catalyst has higher ESA than the other catalysts. The evaluation of a unit cell test using Pt/MWNTs or PtxM(1-x)/MWNTs as the cathode catalysts demonstrated higher cell performance than did a commercial Pt/C catalyst. Among the MWNTs-supported Pt and PtxM(1-x) (M = Co, Cu, Ni) catalysts, the Pt0.77Co0.23/MWNTs shows the highest performance with the cathode catalyst of PEMFC because they had the largest ESA.

Understanding the exact structure and surface characteristics of carbon materials is very important for design, synthesis, and utilization of the best carbon form with particular functions and high performance for practical applications such as selective adsorption adsorbents, energy storage materials, catalysts or catalyst supports, etc. This review paper focuses on carbon surface properties and the interaction between gaseous or liquid substances and carbon surface. Catalytic functions of carbon materials are reviewed including recent progress in synthesis and applications of nano-carbons.

Carbon nanofiber (CNF) grown catalytically was chemically activated with KOH to attain structural change of CNF. The structural changes of CNF through KOH activation were investigated by using BET and SEM. From the results of BET, it was found that KOH activation was effective to develop particular sizes of pores on the CNF surface, increasing the surface area of CNF. Activated CNF was applied as an anode catalyst support of fuel cell. The effects of different activation conditions including the activation temperature and the activation time on the specific surface area of the CNF activated with KOH were investigated to obtain appropriate structure as a catalyst support. The 60 wt% Pt-Ru catalyst prepared was observed by using TEM and XRD.

Direct decomposition of methane over three types of carbon black (N330-p, N330-f, and HI-900L) was carried out in a fluidized bed quartz reactor. Properties of carbon black before and after reaction were measured and found to be related with surface structure and weight gain. For N330-p and N330-f, some carbon deposit on the surface was considered to be the reason for the increase of BET surface area and pore volume with weight gain. Carbon deposits on the surface and the conglutination of some aggregates may explain the slight increase of particle size. Properties of HI-900L changed much more significantly with weight gain. It is supposed that the increase of aggregate size of HI-900L were due to some unknown oily components. The corresponding agglomeration might be the reason for the decrease of BET surface area with weight gain, as compared with the increase of that for the case of N330 black.