Carbon neutrality is one of the central topics of not
only the
scientific community but also the majority of human society. The development
of highly efficient carbon dioxide (CO2) capture and utilization
(CCU) techniques is expected to stimulate routes and concepts to go
beyond fossil fuels and provide more economic benefits for a carbon-neutral
economy. While various single-carbon (C1) and multi-carbon
(C2+) products have been selectively produced to date,
the scope of CCU can be further expanded to more valuable chemicals
beyond simple carbon species by integration of nitrogenous reactants
into CO2 reduction. In this Review, research progress toward
sustainable production of high-value-added chemicals (urea, methylamine,
ethylamine, formamide, acetamide, and glycine) from catalytic
coupling of CO2 and nitrogenous small molecules (NH3, N2, NO3
–, and NO2
–) is highlighted. C–N bond formation
is a key mechanistic step in N-integrated CO2 reduction,
so we focus on the possible pathways of C–N coupling starting
from the CO2 reduction and nitrogenous small molecules
reduction processes as well as the catalytic attributes that enable
the C–N coupling. We also propose research directions and prospects
in the field, aiming to inspire future investigations and achieve
comprehensive improvement of the performance and product scope of
C–N coupling systems.
Aqueous Zn metal batteries have attracted extensive attention due to their intrinsic advantages. However, zinc ions tend to deposit irregularly, seriously depleting the capacity and stability of the battery. The construction of zincophilic sites can effectively regulate the nucleation and growth of Zn, but there is a defect that these sites will be covered with gradual failure after long-term cycling. Here, in combination with the sustained-compensated strategy, interfacial zincophilic sites are continuously constructed, thus effectively avoiding the threat of dendrites and improving the electrochemical performance. Impressively, at 10 mA cm −2 and 5 mAh cm −2 , the protected Zn metal exhibits excellent cycling stability over 2000 cycles in the Zn//Zn battery. Moreover, even the cathode mass loading is considerably high (35 mg cm −2 ), and the Zn//NVO full cell significantly outperforms with high areal capacity (up to 4 mAh cm −2 ). This novel strategy provides a direction for the development of high-capacity aqueous batteries.
Biphasic self-stratified batteries (BSBs) provide a new direction in battery philosophy for large-scale energy storage, which successfully reduces the cost and simplifies the architecture of redox flow batteries. However, current aqueous BSBs have intrinsic limits on the selection range of electrode materials and energy density due to the narrow electrochemical window of water. Thus, herein, we develop nonaqueous BSBs based on Li-S chemistry, which deliver an almost quadruple increase in energy density of 88.5 Wh L−1 as compared with the existing aqueous BSBs systems. In situ spectral characterization and molecular dynamics simulations jointly elucidate that while ensuring the mass transfer of Li+, the positive redox species are strictly confined to the bottom-phase electrolyte. This proof-of-concept of Li-S BSBs pushes the energy densities of BSBs and provides an idea to realize massive-scale energy storage with large capacitance.
Sluggish
desolvation in extremely cold environments caused by strong
Li+–dipole interactions is a key inducement for
the capacity decline of a battery. Although the Li+–dipole
interaction is reduced by increasing the electrolyte concentration,
its high viscosity inevitably limits ion transfer at low temperatures.
Herein, Li+–dipole interactions were eliminated
to accelerate the migration rate of ions in electrolytes and at the
electrode interface via designing Li+–anion nanometric
aggregates (LA-nAGGs) in low-concentration electrolytes. Li+ coordinated by TFSI– and FSI– anions instead of a donor solvent promotes the formation of an inorganic-rich
interfacial layer and facilitates Li+ transfer. Consequently,
the LA-nAGG-type electrolyte demonstrated a high ionic conductivity
(0.6 mS cm–1) at −70 °C and a low activation
energy of charge transfer (38.24 kJ mol–1), enabling
Li||NiFe-Prussian blue derivative cells to deliver ∼83.1% of
their room-temperature capacity at −60 °C. This work provides
an advanced strategy for the development of low-temperature electrolytes.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.