Nitrate Reduction by NiFe-LDH/CeO2: Understanding the Synergistic Effect between Dual-Metal Sites and Dual Adsorption.

Electrocatalytic nitrate reduction reaction (EC-NITRR) shows a significant advantage for green reuse of the nitrate (NO3-) pollutant. However, the slow diffusion reaction limits the reaction rate in practical EC-NITRR, causing an unsatisfactory ammonia (NH3) yield. In this work, a multifunctional NiFe-LDH/CeO2 with the dual adsorption effect (physisorption and chemisorption) and dual-metal sites (Ce3+ and Fe2+) was fabricated by the electrodeposition method. NiFe-LDH/CeO2 performed an expected ability of enrichment for NO3- through the pseudo-first-order and pseudo-second-order kinetic models, and the polymetallic structure provided abundant sites for effective reaction of NO3-. At-0.6 V vs RHE, the ammonia (NH3) yield of NiFe-LDH/CeO2 reached 335.3 µg h-1 cm-2 and the selectivity of NH3 was 24.2 times that of NO2-. The nitrogen source of NH3 was confirmed by 15NO3- isotopic labeling. Therefore, this work achieved the recycling of the NO3- pollutant by synergy of enrichment and catalysis, providing an alternative approach for the recovery of NO3- from wastewater.

Tetrathiafulvalene Carboxylate-Based Anode Material for High-Performance Sodium-Ion Batteries.

Organic electrode materials are promising to be applied in sodium ion batteries (SIBs) due to their low cost and easily modified molecular structures. Nevertheless, low conductivity and high solubility in electrolytes still limit the development of organic electrodes. In this work, a carboxylate small molecule (BDTTS) based on tetrathiafulvalene is developed as anode material for SIBs. BDTTS has a large rigid π-conjugated planar structure, which may reduce solubility in the electrolyte, meanwhile facilitating charge transporting. Experimental results and theoretical calculations both support that apart from the four carbonyl groups, the sulfur atoms on tetrathiafulvalene also provide additional active sites during the discharge/charge process. Therefore, the additional active sites can well compensate for the capacity loss caused by the large molecular weight. The as-synthesized BDTTS electrode renders an excellent capacity of 230 mAh g-1 at a current density of 50 mA g-1 and an excellent long-life performance of 128 mAh g-1 at 2 C after 500 cycles. This work enriches the study on organic electrodes for high-performance SIBs and paves the way for further development and utilization of organic electrodes.

In situ composition of Thienothiophene-based covalent organic framework on carbon nanotube as a host for high performance Li-S batteries.

Lithium-sulfur batteries (LSBs) is a promising secondary battery system with high energy density and environment-friendly characteristics, however, the severe "shuttle effect" and poor conductivity usually lead to short service life and low initial capacity. Carbon Nanotubes (CNTs) with excellent conductivity and large quantity of cavities are promising host materials, whereas, the weak interaction between CNTs and polysulfides usually leads to serious shuttle effect in charge/discharge processes. Herein, thienothiophene-based covalent organic framework is uniformly wrapped on the outer surface of CNTs to form a nanocomposite TT-BOST@CNT. It is observed that the coexistence of the electron-rich S, O and the electron-deficient B atoms enables the effective adsorption of both Li+ and Sx2- in lithium polysulfides (LiPSs). Studies reveal that the B, O and S atoms endow the nanocomposite with good catalysis ability, whereby, conversion of the insoluble long-chain polysulfides to the soluble short-chain polysulfides is accelerated. Consequently, the TT-BOST@CNT/S cathode displays outstanding electrochemical performance, with a high discharge specific capacity of 1545 mAh g-1 at 0.2 C and a small attenuation rate of 0.035% per cycle in 1000 cycles at 1 C.

Adjusting morphological properties of organic electrode material for efficient Sodium-ion batteries by isomers strategy.

In this work, two isomers are mixed in different proportions and then alkalized as the organic anode material for sodium-ion batteries (SIBs). The mixed material, denoted as PN, shows distinct morphology and electrochemical properties, compared to the single-component Na-CPP and Na-CPN. The Initial Coulombic Efficiency (ICE) value obtained by using the mixed PN as anode is higher than that using the single component. And the capacity retention rate of the mixed PN electrode is 92% after 1200 cycles under 935 mA g-1 high current density. This is mainly due to the superior morphology of the mixed PN electrode (the optimal ratio is CPP: CPN = 3: 1, the mass ratio (or molar ratio)), which exhibits more uniform spherical particles, thus increasing the contact area with the electrolyte and ensuring close contact with the conductive carbon. As a result, the ICE and cycle performance is improved because of the reduced irreversible side reactions. As far as we know, this is the first example of mixing two isomers as organic anode materials in traditional SIBs, and this strategy may provide new insights into future development of organic electrode materials.

Phenylpyridine Dicarboxylate as Highly Efficient Organic Anode for Na-Ion Batteries.

The sodium-ion battery (SIB) has the potential to be the next-generation rechargeable system, utilizing cheap and abundant sodium material. One of the key obstacles to sodium batteries is the lack of efficient and stable anode materials. Compared with traditional inorganic electrode materials, organic materials are more attractive because of their easier sodium transport accessibility and the diversities of organic frameworks and functional groups. In this work, two molecules (Na-CPN and Na-CPP) were synthesized and used as anode materials for SIBs. Structurally, the two compounds are isomers, and they are distinguished by the position of N atoms in phenylpyridine. Na-CPP showed a high reversible capacity of 197 mAh g-1 , and its capacity could maintain 99.1 % of its initial value even after 350 cycles of 100 mA g-1 . Moreover, after going through 1200 cycles at a current density of 5 C, the Na-CPP electrode still retained a capacity rate of 89.9 %. In contrast, Na-CPN exhibited inferior capacity and rate performance because of its larger polarization, particle size, and charge transport resistance.