Nickel (Ni)-lignin nanocomposites were synthesized from nickel nitrate and kraft lignin then catalytically graphitized to few-layer graphene-encapsulated nickel nanoparticles ([email protected]). [email protected] nanoparticles were used for catalytic decomposition of methane (CDM) to produce COx-free hydrogen and graphene nanoplatelets. [email protected] showed high catalytic activity for methane decomposition at temperatures of 800 to 900 °C and exhibited long-term stability of 600 min time-on-stream (TOS) without apparent deactivation. The catalytic stability may be attributed to the nickel dispersion in the [email protected] sample. During the CDM reaction process, graphene shells over [email protected] nanoparticles were cracked and peeled off the nickel cores at high temperature. Both the exposed nickel nanoparticles and the cracked graphene shells may participate the CDM reaction, making [email protected] samples highly active for CDM reaction. The vacancy defects and edges in the cracked graphene shells serve as the active sites for methane decomposition. The edges are continuously regenerated by methane molecules through CDM reaction.
For fuel cells, to produce high-quality and low-platinum catalyst is a pressing technical problem. In this study, graphene cathode catalysts with controllable platinum content were decorated by pyrolyzing chloroplatinic acid under various process parameters to obtain a high catalytic activity and durability. The results show that platinum particles generated by pyrolyzing chloroplatinic acid are uniformly loaded on graphene without agglomeration. The average particle size of platinum particles is about 2.12 nm. The oxygen reduction reaction catalytic activity of catalyst samples first increases, then decreases with increasing platinum loading in cyclic voltammetry and LSV. Compared with the commercial Pt/C (20 wt% Pt) catalyst, the initial potential and the current density retention rate of the catalyst decorated with 8% platinum are 55 mV and 23.7% higher, respectively. From i-t curves, it was found that the stability of the catalyst prepared in this paper was improved compared with the commercial Pt/C catalyst. The catalysts prepared in the present research exhibits superior catalytic activity and stability.
The Fenton-like process catalyzed by metal-free materials presents one of the most promising strategies to deal with the ever-growing environmental pollution. However, to develop improved catalysts with adequate activity, complicated preparation/modification processes and harsh conditions are always needed. Herein, we proposed an ultrafast and facile strategy to convert various inefficient commercial nanocarbons into highly active catalysts by noncovalent functionalization with polyethylenimine (PEI). The modified catalysts could be in situ fabricated by direct addition of PEI aqueous solution into the nanocarbon suspensions within 30 s and without any tedious treatment. The unexpectedly high catalytic activity is even superior to that of the single-atom catalyst and could reach as high as 400 times higher than the pristine carbon material. Theoretical and experimental results reveal that PEI creates net negative charge via intermolecular charge transfer, rendering the catalyst higher persulfate activation efficiency.
Solid supports functionalized with molecular metal catalysts combine many of the advantages of heterogeneous and homogeneous catalysis. A (NNN)Ru-incorporated porous organic polymer (POP-bp/bbpRuCl3) exhibited high catalytic efficiency and broad functional group tolerance in the C–C cross-coupling of secondary and primary alcohols to give β-alkylated secondary alcohols. This catalyst demonstrated excellent durability during successive recycling without leaching of Ru which is ascribed to the strong binding of the pincer ligands to the metal ions.
The synthesis of metal-free carbon-based electrocatalysts for oxygen reduction reactions (ORR) to replace conventional Pt-based catalysts has become a hot spot in current research. This work proposes an activation-assisted carbonization strategy, to manufacture N-doped ultra-thin carbon nanosheets (GWS180M800) with high catalytic activity, namely, melamine is used as an accelerator/nitrogen source, and walnut green peels biological waste as a carbon source. The melamine acts as a nitrogen donor in the hydrothermal process, effectively enhancing the nitrogen doping rate. The content of pyridine nitrogen groups accounts for up to 48.5% of the total nitrogen content. Electrochemical tests show that the GWS180M800 has excellent ORR electrocatalytic activity and stability, and makes a quasi-four-electron ORR pathway clear in the alkaline electrolyte. The initial potential and half slope potential are as high as 1.01 and 0.82 V vs. RHE, respectively. The GWS180M800 catalyst has a better ability to avoid methanol cross poisoning than Pt/C has. Compared with 20 wt% Pt/C, GWS180M800 has improved methanol tolerance and stability. It is a metal-free biochar ORR catalyst with great development potential and application prospects. This result provides a new space for the preparation of valuable porous nano-carbon materials based on carbonaceous solid waste and provides new ideas for catalyzing a wide range of electrochemical reactions in the future.
Fuel cells are a key enabling technology for the future economy, thereby providing power to portable, stationary, and transportation applications, which can be considered an important contributor towards reducing the high dependencies on fossil fuels. Electrocatalyst plays a vital role in improving the performance of the low temperature fuel cells. Noble metals (Pt, Pd) supported on carbon have shown promising performance owing to their high catalytic activity for both electroreduction and electrooxidation and have good stability. Catalyst preparation by electrodeposition is considered to be simple in terms of operation and scalability with relatively low cost to obtain high purity metal deposits. This review emphasises the role of electrodeposition as a cost-effective method for synthesising fuel cell catalysts, summarising the progress in the electrodeposited Pt and Pd catalysts for direct liquid fuel cells (DLFCs). Moreover, this review also discusses the technological advances made utilising these catalysts in the past three decades, and the factors that impede the technological advancement of the electrodeposition process are presented. The challenges and the fundamental research strategies needed to achieve the commercial potential of electrodeposition as an economical, efficient methodology for synthesising fuel cells catalysts are outlined with the necessary raw materials considering current and future savings scenario.
Exploring and fabricating a suitable photoanode with high catalytic activity is critical for enhancing photoelectrochemical (PEC) performance. Herein, a novel 3D hierarchical Fe2O3/SnO2 photoanode was fabricated by a hydrothermal route, combining with an annealing process. The morphology, crystal structure were studied by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photon spectroscopy (XPS), and X-ray diffraction (XRD), respectively. The results reveal the successful preparation of Fe2O3 nanothorns on the surface of SnO2 nanosheets. The as-fabricated 3D Fe2O3/SnO2 photoanode yields obviously promoted PEC performance with a photocurrent density of approximate 5.85 mA cm-2, measured in a mixture of Na2S (0.25 M) and Na2SO3 (0.35 M) aqueous solution at 1.23 V (vs. reversible hydrogen electrode, RHE). This value of photocurrent is about 53 times higher than that of the bare SnO2 photoanode. The obvious improved PEC properties can be attributed to the 3D Fe2O3/SnO2 heterostructures that offer outstanding light harvesting ability as well as improved charge transport and separation. These results suggest that exploring a suitable 3D hierarchical photoanode is an effective approach to boost PEC performance.approach to boost PEC performance.
AbstractThe use of magnetic nanoparticles in C–C coupling reactions enables the facile recovery of the catalyst under environmentally friendly conditions. Herein, the synthesis of Pd/[email protected] nanoparticles by the reduction of Pd2+ and oxidation of Fe on the surface of preformed [email protected] is reported. The nanoparticles were characterized using a variety of analytical techniques (transmission electron microscopy, Mössbauer spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction) to determine their size, structure, and chemical composition. The catalytic efficiency of these nanoparticles in classical Suzuki–Miyaura coupling reactions was investigated. The nanoparticles achieved high catalytic activity with the application of local heating by an alternating magnetic field. An investigation was conducted at identical temperatures to compare global heating with the application of an external magnetic field; magnetic heating demonstrated excellent substrate conversion in lesser time and at a lower temperature. The catalyst could also be recycled and reused three times, with ~ 30% decrease in the substrate conversion, which is most likely due to the agglomeration of the Pd nanoparticles or poisoning of the Pd catalyst. This approach, which takes advantage of the catalytic activity and magnetic susceptibility of magnetic nanoparticles, can be applied to several organic transformations to improve their efficiency.
Direct CO2 hydrogenation to long-chain hydrocarbons can mitigate global warming by extensively replacing fossil fuels. However, designing a suitable catalyst with high catalytic activity and C5+ hydrocarbon selectivity continues to...