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Exploring high efficient and cost-effective electrocatalysts for oxygen evolution reaction is a determination step towards sustainable green energy applications. Polyoxometalates and layered double hydroxide materials are suggested to be potential catalyst materials; however, those electrocatalytic behaviors are greatly inferior to the state-of-the-art OER electrocatalysts (RuO2 and IrO2). In this work, we employ a self-assembly approach in which polyoxometalate anions are successfully intercalated into NiFe layered double hydroxide. Upon analysis of the composition, the elemental valence state and the infrared spectrum, it confirms that the intercalated polyoxometalate anions in the layers of NiFe layered double hydroxide are in the format of PW12O403−. Even though the partial anions in the as-prepared intercalation NiFe layered double hydroxide are only polyoxometalate anions, its electrochemical performance surpasses the counterpart precursor NiFe layered double hydroxide (NO3−) in many aspects, such as turnover frequencies, overpotentials, kinetics, and stability. The introduction of polyoxometalate anions can optimize the local electronic structure which enhances the charge transport capacity of NiFe layered double hydroxide as well as alter the adsorption/desorption nature of the intermediates during the catalysis process. This work provides a new strategy to boost the OER activity of layered double hydroxide-based electrocatalysts.

Defect engineering has been used to develop low-cost and effective catalysts to boost oxygen reduction reactions. However, the development of catalysts that use metal cation vacancies as the active sites for oxygen reduction reaction is lacking. In this study, ZnS nanoparticles on N-doped carbon serve as an oxygen reduction reaction catalyst. These catalysts were prepared via a one-step method at 900 °C. Amazingly, the high-resolution transmission electron microscope image revealed obvious defects in the ZnS nanoparticles. These facilitated the catalyst synthesis, and the product displayed good electrocatalytic performance for the oxygen reduction reaction in an alkaline medium, including a lower onset potential, lower mid-wave potential, four electron transfer process, and better durability compared with 20 wt% Pt/C. More importantly, the density functional theory results indicated that using the Zn vacancies in the prepared catalyst as active sites required a lower reaction energy to produce OOH* from *OO toward oxygen reduction reaction. Therefore, the proposed catalyst with Zn vacancies can be used as a potential electrocatalyst and may be substitutes for Pt-based catalysts in fuel cells, given the novel catalyst's resulting performance.

Fe-based carbon materials are widely considered promising to replace Pt/C as next-generation electrocatalysts towards oxygen reduction reaction (ORR). However, the preparation of Fe-based carbon materials is still carried out by conventional heating method (CHM). Herein, a novel microwave-assisted carbon bath method (MW-CBM) was proposed, which only took 35 min to synthesize Fe/Fe3C nanoparticles encapsulated in N-doped carbon layers derived from Prussian blue (PB). The catalyst contained large specific surface area and mesoporous structure, abundant Fe-Nx and CN active sites, unique core-shell structure. Due to the synergistic effects of these features, the as-prepared Fe/Fe3C@NC-2 displayed outstanding ORR activity with onset potential of 0.98 VRHE and half-wave potential of 0.87 VRHE, which were more positive than 20 wt.% Pt/C (0.93 VRHE and 0.82 VRHE). Besides, Fe/Fe3C@NC-2 gave a better stability and methanol tolerance than Pt/C towards ORR in alkaline media, too. Keywords: Fe/Fe3C nanoparticles, Prussian blue, Microwave, Carbon bath method, Oxygen reduction reaction

High active and durable non-noble metal electrocatalysts are urgently developed to satisfy the high performance oxygen reduction reaction (ORR). We successfully synthesized Co-CoOx anchored on nitrogen-doped carbon via a facile sand-bath method (SBM), i.e., Co-CoOx/N-C (SBM). The as-obtained Co-CoOx/N-C (SBM) exhibited overwhelming superiorities to Co-CoO/N-C prepared by conventional heat treatment (CHT), particularly in electrochemical performance of ORR. Although Co-CoOx/N-C (SBM) showed smaller specific surface area of 276.8 m2/g than that of 939.5 m2/g from Co-CoO/N-C (CHT), the Co-CoOx/N-C (SBM) performed larger pore diameter and more Co3O4 active component resulting in better ORR performance in 0.1 mol/L KOH solution. The Co-CoOx/N-C (SBM) delivered onset potential of 0.91 V vs. RHE, mid-wave potential of 0.85 V vs. RHE and limited current density of 5.46 mA/cm2 much better than those of the Co-CoO/N-C (CHT). Furthermore, Co-CoOx/N-C (SBM) showed greater stability and better methanol tolerance superior to the commercial 20 wt% Pt/C.

In this paper, we developed a simple two-step route to prepare a PdO/SnO2 heterostructure with the diameter of the SnO2 and PdO nanoparticles at about 15 nm and 3 nm, respectively. In the evaluation temperature window between 80 °C and 340 °C, PdO/SnO2 shows the best response to 100 ppm of CO at 100 °C with fast response time (14 s) and recovery time (8 s). Furthermore, the PdO/SnO2 nanoparticles exhibit a low detection limit and good selectivity to CO against interfering gases as well as rarely-seen low-temperature stability and reversibility. Such enhanced gas sensing performance could be attributed to both the ultrafine structure of PdO and the synergy between PdO and SnO2. The results clearly indicate the application of PdO/SnO2 as a pratical low-temperature sensing material for CO.

The rapid emergence of graphene has attracted numerous efforts to explore other two-dimensional materials. Here, we combine first-principles calculations and Boltzmann theory to investigate the structural, electronic, and thermoelectric transport properties of monolayer C3N, which exhibits a honeycomb structure very similar to graphene. It is found that the system is both dynamically and thermally stable even at high temperature. Unlike graphene, the monolayer has an indirect band gap of 0.38 eV and much lower lattice thermal conductivity. Moreover, the system exhibits obviously larger electrical conductivity and Seebeck coefficients for the hole carriers. Consequently, the ZT value of p-type C3N can reach 1.4 at 1200 K when a constant relaxation time is predicted by the simple deformation potential theory. However, such a larger ZT is reduced to 0.6 if we fully consider the electron–phonon coupling. Even so, the thermoelectric performance of monolayer C3N is still significantly enhanced compared with that of graphene, and is surprisingly good for low-dimensional thermoelectric materials consisting of very light elements.

Electrocatalysts with strong stability and high electrocatalytic activity have received increasing interest for oxygen reduction reactions (ORRs) in the cathodes of energy storage and conversion devices, such as fuel cells and metal-air batteries. However, there are still several bottleneck problems concerning stability, efficiency, and cost, which prevent the development of ORR catalysts. Herein, we prepared bimetal FeCo alloy nanoparticles wrapped in Nitrogen (N)-doped graphitic carbon, using Co-Fe Prussian blue analogs (Co3[Fe(CN)6]2, Co-Fe PBA) by the microwave-assisted carbon bath method (MW-CBM) as a precursor, followed by dielectric barrier discharge (DBD) plasma treatment. This novel preparation strategy not only possessed a fast synthesis rate by MW-CBM, but also caused an increase in defect sites by DBD plasma treatment. It is believed that the co-existence of Fe/Co-N sites, rich active sites, core-shell structure, and FeCo alloys could jointly enhance the catalytic activity of ORRs. The obtained catalyst exhibited a positive half-wave potential of 0.88 V vs. reversible hydrogen electrode (RHE) and an onset potential of 0.95 V vs. RHE for ORRs. The catalyst showed a higher selectivity and long-term stability than Pt/C towards ORR in alkaline media.

Half-Heusler compounds usually exhibit relatively higher lattice thermal conductivity that is undesirable for thermoelectric applications. Here we demonstrate by first-principles calculations and Boltzmann transport theory that the BiBaK system is an exception, which has rather low thermal conductivity as evidenced by very small phonon group velocity and relaxation time. Detailed analysis indicates that the heavy Bi and Ba atoms form a cage-like structure, inside which the light K atom rattles with larger atomic displacement parameters. In combination with its good electronic transport properties, the BiBaK shows a maximum n-type ZT value of 1.9 at 900 K, which outperforms most half-Heusler thermoelectric materials.