ABSTRACT
Unraveling the configuration-activity relationship and synergistic enhancement mechanism (such as real active center, electron spin-state, and d-orbital energy level) for triatomic catalysts, as well as their intrinsically bifunctional oxygen electrocatalysis, is a great challenge. Here we present a triatomic catalyst (TAC) with a trinuclear active structure that displays extraordinary oxygen electrocatalysis for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), greatly outperforming the counterpart of single-atom and diatomic catalysts. The aqueous Zn-air battery (ZAB) equipped with a TAC-based cathode exhibits extraordinary rechargeable stability and ultrarobust cycling performance (1970 h/3940 cycles at 2 mA cm-2, 125 h/250 cycles at 10 mA cm-2 with negligible voltage decay), and the quasi-solid-state ZAB displays outstanding rechargeability and low-temperature adaptability (300 h/1800 cycles at 2 mA cm-2 at -60 °C), outperforming other state-of-the-art ZABs. The experimental and theoretical analyses reveal the symmetry-breaking CoN4 configuration under incorporation of neighboring metal atoms (Fe and Cu), which leads to d-orbital modulation, a low-shift d band center, weakened binding strength to the oxygen intermediates, and decreased energy barrier for bifunctional oxygen electrocatalysis. This rational tricoordination design as well as an in-depth mechanism analysis indicate that hetero-TACs can be promisingly applied in various electrocatalysis applications.
ABSTRACT
The rapid development of portable and wearable electronics has given rise to new challenges and provoked research in flexible, lightweight, and affordable energy storage devices. Flexible solid-state metal-air batteries (FSSMABs) are considered promising candidates, owing to their large energy density, mechanical flexibility, and durability. However, the practical applications of FSSMABs require further improvement to meet the demands of long-term stability, high power density, and large operating voltage. This Review presents a detailed discussion of innovative electrocatalysts for the air cathode, followed by a sequential overview of high-performance solid-state electrolytes and metal anodes, and a summary of the current challenges and future perspectives of FSSMABs to promote practical application and large-scale commercialization in the near future.
ABSTRACT
Ansalactam A is an ansa macrolide natural product that contains a densely functionalized spiro-γ-lactam core containing three contiguous stereocenters. This unusual motif distinguishes it from other members of this family and represents a significant synthetic challenge. Herein, we report the development of a stereoselective formal [3+2] cycloaddition reaction for the construction of this key spiro-γ-lactam motif for the first time, thereby enabling access to the northern domain of ansalactam A.
Subject(s)
Spiro CompoundsABSTRACT
Global climate change and socio-economic development have led to a shortage of water and labour resources, which has had a significant impact on rice cultivation. In this study, the application of micro-ridge-furrow planting technology and degradable film mulching in dry direct-seeded rice was investigated to address the factors restricting the development of the rice industry and reduce the impact of rice production on the environment. The effects of a micro-ridge-furrow planting pattern and degradable film mulching on soil temperature, seedling growth, and yield of dry direct-seeded rice in a semiarid region of China were studied through three field experiments: micro-ridge-furrow mulching with traditional plastic film (T1); micro-ridge-furrow mulching with degradable film (T2); and traditional flat-cropping mulching with traditional plastic film (CK). The experimental results demonstrated that the micro-ridge-furrow mulching film planting pattern promoted the germination of rice seeds and improved the soil temperature, plant height, leaf area, dry mass, and grain yield. T2 had the highest average soil temperature (14.68-17.83 â during the day; 14.4-15.74 â at night), leaf area (41.85 cm2 plant-1), root dry mass (45.32 mg plant-1), shoot dry mass (58.46 mg plant-1), root-shoot ratio (0.821), and yield (8.112 t ha-1). In summary, the micro-ridge-furrow mulching with degradable film (T2) is recommended as an efficient planting and mulching pattern for sustainably solving environmental problems and improving grain yield in semiarid regions of China.
ABSTRACT
A concise, protecting-group-free total synthesis of the unusual brominated sesquiterpene aplydactone is described. Our synthesis features a [2+2] photocycloaddition, a Wolff ring contraction, an unusual remote C-H functionalization to establish the highly strained tetracyclic core, and a hydrogen-atom transfer (HAT) reaction to access the bromine-containing stereocenter. A finely tuned conformation of the α-diazoketone precursor is the key for the success of the late-stage transannular C-H insertion to deliver a bridged six-membered ring and a quaternary stereocenter (C6) between two quaternary carbon atoms (C1 and C7).
