Tailoring the electronic arrangement of graphene by doping is a practical strategy for producing significantly improved materials for the oxygen-reduction reaction (ORR) in fuel cells (FCs). Recent studies have proven that the carbon materials doped with the elements, which have the larger (N) or smaller (P, B) electronegative atoms than carbon such as N-doped carbon nanotubes (CNTs), P-doped graphite layers and B-doped CNTs, have also shown pronounced catalytic activity. Herein, we find that the graphenes doped with the elements, which have the similar electronegativity with carbon such as sulfur and selenium, can also exhibit better catalytic activity than the commercial Pt/C in alkaline media, indicating that these doped graphenes hold great potential for a substitute for Pt-based catalysts in FCs. The experimental results are believed to be significant because they not only give further insight into the ORR mechanism of these metal-free doped carbon materials, but also open a way to fabricate other new low-cost NPMCs with high electrocatalytic activity by a simple, economical, and scalable approach for real FC applications.

An integrated, selective interlayer structure is developed to further mitigate the diffusion of polysulfides, simply by coating the surface of a C–S cathode with a graphene/TiO2 film. It is found that the application of the graphene/TiO2 film as an interlayer enables the porous carbon nanotubes–S cathode to exhibit a high reversible specific capacity and extraordinarily excellent cycling stability.

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Iodine-doped graphene has been successfully fabricated through a simple, economical, and scalable approach. The new metal-free catalyst can exhibit a high catalytic activity, long-term stability, and an excellent methanol tolerance for the oxygen reduction reaction.

Despite the good progress in developing doped carbon catalysts for oxygen-reduction reaction (ORR), the current metal-free carbon catalysts are still far from satisfactory for large-scale applications of fuel cell. Developing new metal free doped carbon materials with abundance active sites as well as excellent electron transfer and reactant transport rate towards ORR may be a potential solution. Herein, we develop a novel three-dimensional (3D) sulfur-nitrogen co-doped carbon foams (S-N-CF) with hierarchical pore structures, using a convenient, economical, and scalable method. The experimental results have demonstrated that the obtained 3D S-N-CF exhibited better catalytic activity, longer-term stability and higher methanol tolerance than a commercial Pt/C catalyst. Such excellent performances may be attributed to the synergistic effect, which includes high catalytic sites for ORR provided by high S-N heteroatom loading, excellent reactant transport caused by hierarchical pore structures and high electron transfer rate provided by 3D continuous networks. Our results not only develop a new type of catalysts with excellent electrocatalytic performance by a commercially valid route, but also provide useful information for further clarification of the relationship between the microstructures of metal-free carbon materials and catalyst properties for ORR. More importantly, the idea to design hierarchical pore structures could be applied to other catalytic materials and serve as a general strategy for improving the activity of various ORR catalysts.

The ongoing search for new non-precious-metal catalysts (NPMCs) with excellent electrocatalytic performance to replace Pt-based catalysts has been viewed as an important strategy to promote the development of fuel cells. Recent studies have proven that carbon materials doped with atoms which have a relatively small atomic size (e.g. N, B, P or S), have also shown pronounced catalytic activity. Herein, we demonstrate the successful fabrication of CNT/graphene doped with Se atoms, which has a relatively large atomic size, by a simple, economical, and scalable approach. The electrocatalytic performance of the resulting Se-doped CNT-graphene catalyst exhibits excellent catalytic activity, long-term stability, and a high methanol tolerance compared to commercial Pt/C catalysts. Our results confirmed that combining CNTs with graphene is an effective strategy to synergistically improve ORR activity. More importantly, it is also suggested that the development of graphite materials doped with Se or other heteroatoms of large size will open up a new route to obtain ideal NPMCs with realistic value for fuel cell applications.

Lithium-sulfur batteries have become an appealing candidate for next-generation energy-storage technologies because of their low cost and high energy density. However, one of their major practical problems is the high solubility of long-chain lithium polysulfides and their infamous shuttle effect, which causes low Coulombic efficiency and sulfur loss. Here, we introduced a concept involving the dithiothreitol (DTT) assisted scission of polysulfides into lithium-sulfur system. Our designed porous carbon nanotube/S cathode coupling with a lightweight graphene/DTT interlayer (PCNTs-S@Gra/DTT) exhibited ultrahigh cycle-ability even at 5 C over 1100 cycles, with a capacity degradation rate of 0.036% per cycle. Additionally, the PCNTs-S@Gra/DTT electrode with a 3.51 mg cm sulfur mass loading delivered a high initial areal capacity of 5.29 mAh cm (1509 mAh g) at current density of 0.58 mA cm, and the reversible areal capacity of the cell was maintained at 3.45 mAh cm (984 mAh g) over 200 cycles at a higher current density of 1.17 mA cm. Employing this molecule scission principle offers a promising avenue to achieve high-performance lithium-sulfur batteries.

A novel electrochemical sensor was developed for sensitive and selective detection of mercury(II), based on thymine-Hg2+-thymine (T-Hg2+-T) coordination chemistry. This strategy exploited the cooperativity of proximate poly-T oligonucleotides in coordination with Hg2+. Ferrocene (Fc)-tagged poly-T oligonucleotides were immobilized on the electrode surface via self-assembly of the terminal thiol moiety. In the presence of Hg2+, a pair of poly-T oligonucleotides could cooperatively coordinate with Hg2+, which triggered a conformational reorganization of the poly-T oligonucleotides from flexible single strands to relatively rigid duplexlike complexes, thus drawing the Fc tags away from the electrode with a substantially decreased redox current. The response characteristics of the sensor were thoroughly investigated using capillary electrophoresis and electrochemical measurements. The results revealed that the sensor showed a sensitive response to Hg2+ in a concentration range from 1.0 nM to 2.0 microM, with a detection limit of 0.5 nM. Also, this strategy afforded exquisite selectivity for Hg2+ against a reservoir of other environmentally related metal ions, compared to existing anodic stripping voltammetry (ASV) techniques. In addition, this sensor could be implemented using minimal reagents and working steps with excellent reusability through mild regeneration procedure. It was expected that this cost-effective electrochemical sensor might hold considerable potential in on-site applications of Hg2+ detection.