The Enhancement Mechanism of Different Single-Transition Metal Atomic Catalysts/Sulfur Cathode on High-Performance of Li-S Batteries.

Materials with various single-transition metal atoms dispersed in nitrogenated carbons (M─N─C, M = Fe, Co, and Ni) are synthesized as cathodes to investigate the electrocatalytic behaviors focusing on their enhancement mechanism for performance of Li-S batteries. Results indicate that the order of both electrocatalytic activity and rate capacity for the M─N─C catalysts is Co > Ni > Fe, and the Co─N─C delivers the highest capacity of 1100 mAh g-1 at 1 C and longtime stability at a decay rate of 0.05% per cycle for 1000 cycles, demonstrating excellent battery performance. Theoretical calculations for the first time reveal that M─N─N─C catalysts enable direct conversion of Li2 S6 to Li2 S rather than Li2 S4 to Li2 S by stronger adsorption with Li2 S6 , which also has an order of Co > Ni > Fe. And Co─N─C has the strongest adsorption energy, not only rendering the highest electrocatalytic activity, but also depressing the polysulfides' dissolution into electrolyte for the longest cycle life. This work offers an avenue to design the next generation of highly efficient sulfur cathodes for high-performance Li-S batteries, while shedding light on the fundamental insight of single metal atomic catalytic effects on Li-S batteries.

Stabilizing Single-Atomic Pt by Forming PtFe Bonds for Efficient Diboration of Alkynes.

Precisely tailoring the oxidation state of single-atomic metal in heterogeneous catalysis is an efficient way to stabilize the single-atomic site and promote their activity, but realizing this approach remains a grand challenge to date. Herein, a class of stable single-atomic catalysts with well-tuned oxidation state of Pt by forming PtFe atomic bonds is reported, which are supported by defective Fe2 O3  nanosheets on reduced graphene oxide (PFARFNs). These as-synthesized materials can greatly enhance the catalytic activity, stability, and selectivity for the diboration of alkynes. The PFARFNs exhibit high conversion of 99% at 100 °C with an outstanding turnover frequency (TOF) of 545 h-1 , and a relatively high conversion of 58% at room temperature (25 °C) with a TOF of 310 h-1 , which has been hardly achieved previously. Through both experimental and theoretical investigation, it is demonstrated that the fast electron transfer from Fe to Pt in Fe-Pt-O atomic sites in PFARFNs can not only stabilize the single-atomic Pt, but also significantly improve their catalytic activity.

Co2+ anchored on surface-functionalized PET non-woven fabric and used as high efficiency monoatom-like catalyst for activating Oxone in water.

Fenton-like processes have emerged as most promising techniques for generating reactive oxygen-containing radicals to deal with increasing levels of environmental pollution. Developing novel catalysts with simple manufacturing requirements, excellent activity levels, and stability remains a long-term goal in terms of practical application. So herein, a new polyethylene terephthalate (PET) non-woven fabric based composite catalyst has been fabricated, using radiation-induced graft polymerization of a functionalized group to chelate Co2+ ions as heterogeneous catalysts in peroxymonosulfate (Oxone) activation. Several impact factors, including catalyst dosage, Oxone concentration, reaction temperature, pH value, Co2+ precipitation ratio (of Co@PET at different pH values), and highly concentrated NaCl have been investigated here. Notably, Co@PET has shown the lowest activation energy of any reported catalyst, for degrading RhB by activating Oxone. Interestingly, as experimental RhB and Oxone solutions were passed through single Co@PET sheets, the RhB was decomposed into a colorless solution in the penetration process. Based on radical trapping and quenching experiments, a channel was determined to dominate RhB degradation, and furthermore, Co@PET could be re-used for RhB degradation by activating Oxone. These results showed that Co@PET effectively provided improved Fenton-like catalytic performance and stability, and was suitable for practical applications.

Atomic Iron Catalysis of Polysulfide Conversion in Lithium-Sulfur Batteries.

Lithium-sulfur batteries have been regarded as promising candidates for energy storage because of their high energy density and low cost. It is a main challenge to develop long-term cycling stability battery. Here, a catalytic strategy is presented to accelerate reversible transformation of sulfur and its discharge products in lithium-sulfur batteries. This is achieved with single-atomic iron active sites in porous nitrogen-doped carbon, prepared by polymerizing and carbonizing diphenylamine in the presence of iron phthalocyanine and a hard template. The Fe-PNC/S composite electrode exhibited a high discharge capacity (427 mAh g-1) at a 0.1 C rate after 300 cycles with the Columbic efficiency of above 95.6%. Besides, the electrode delivers much higher capacity of 557.4 mAh g-1 at 0.5 C over 300 cycles. Importantly, the Fe-PCN/S has a smaller phase nucleation overpotential of polysulfides than nitrogen-doped carbon alone for the formation of nanoscale of Li2S as revealed by ex situ SEM, which enhance lithium-ion diffusion in Li2S, and therefore a high rate performance and remarkable cycle life of Li-sulfur batteries were achieved. Our strategy paves a new way for polysulfide conversion with atomic iron catalysis to exploit high-performance lithium-sulfur batteries.