The abundant reserve and low cost of sodium have provoked tremendous evolution of Na-ion batteries (SIBs) in the past few years, but their performances are still limited by either the specific capacity or rate capability. Attempts to pursue high rate ability with maintained high capacity in a single electrode remains even more challenging. Here, an elaborate self-branched 2D SnS (B-SnS) nanoarray electrode is designed by a facile hot bath method for Na storage. This interesting electrode exhibits areal reversible capacity of ca. 3.7 mAh cm (900 mAh g) and rate capability of 1.6 mAh cm (400 mAh g) at 40 mA cm (10 A g). Improved extrinsic pseudocapacitive contribution is demonstrated as the origin of fast kinetics of an alloying-based SnS electrode. Sodiation dynamics analysis based on first-principles calculations, ex-situ HRTEM, in situ impedance, and in situ Raman technologies verify the S-edge effect on the fast Na migration and reversible and sensitive structure evolution during high-rate charge/discharge. The excellent alloying-based pseudocapacitance and unsaturated edge effect enabled by self-branched surface nanoengineering could be a promising strategy for promoting development of SIBs with both high capacity and high rate response.
Surface organic ligands playac ritical role in stabilizing atomically precise metal nanoclusters in solutions. However,itisstill challenging to prepare highly robust ligated metal nanoclusters that are surface-active for liquid-phase catalysis without any pre-treatment. Now,a nN -heterocyclic carbene-stabilized Au 25 nanocluster with high thermal and air stabilities is presented as ah omogenous catalyst for cycloisomerization of alkynyl amines to indoles.T he nanocluster, characterized as [Au 25 ( i Pr 2 -bimy) 10 Br 7 ] 2+ ( i Pr 2 -bimy = 1,3-diisopropylbenzimidazolin-2-ylidene) (1), was synthesized by direct reduction of AuSMe 2 Cl and i Pr 2 -bimyAuBr with NaBH 4 in one pot. X-rayc rystallization analysis revealed that the cluster comprises two centered Au 13 icosahedra sharing av ertex. Cluster 1 is highly stable and can survive in solution at 80 8 8Cf or 12 h, which is superior to Au 25 nanoclusters passivated with phosphines or thiols.DFT computations reveal the origins of both electronic and thermal stability of 1 and point to the probable catalytic sites.T his work provides new insights into the bonding capability of N-heterocyclic carbene to Au in ac luster,a nd offers an opportunity to probe the catalytic mechanism at the atomic level.
Owing
to the ionic nature of lead halide perovskites, their halide-terminated
surface is unstable under light-, thermal-, moisture-, or electric-field-driven
stresses, resulting in the formation of unfavorable surface defects.
As a result, nonradiative recombination generally occurs on perovskite
films and deteriorates the efficiency, stability, and hysteresis performances
of perovskite solar cells (PSCs). Here, a surface iodide management
strategy was developed through the use of cesium sulfonate to stabilize
the perovskite surface. It was found that the pristine surface of
common perovskite was terminated with extra iodide, that is, with
an I–/Pb2+ ratio larger than 3, explaining
the origination of surface-related problems. Through post-treatment
of perovskite films by cesium sulfonate, the extra iodide on the surface
was facilely removed and the as-exposed Pb2+ cations were
chelated with sulfonate anions while maintaining the original 3D perovskite
structure. Such iodide replacement and lead chelating coordination
on perovskite could reduce the commonly existing surface defects and
nonradiative recombination, enabling assembled PSCs with an efficiency
of 22.06% in 0.12 cm2 cells and 18.1% in 36 cm2 modules with high stability.
The complexity of heterogeneous metal
catalysts makes it challenging
to gain insights into their catalytic mechanisms. Thus, there exists
a huge gap between heterogeneous catalysis and organometallic catalysis.
With the success in the preparation of highly robust atomically precise
metal nanocluster catalysts (i.e., [Au16(NHC-1)5(PA)3Br2]3+ and [Au17(NHC-1)4(PA)4Br4]+, where
NHC-1 is a bidentate NHC ligand, and PA is phenylacetylide) with surface
organometallic motifs anchored on the metallic core, we demonstrate
in this work how the metallic core works synergistically with the
surface organometallic motifs to enhance the catalysis. More importantly,
the discovery allows the development of highly stable and recyclable
heterogeneous metal catalysts to achieve efficient hydroamination
of alkynes with an extremely low catalyst dosage (0.002 mol %), helping
bridge the gap between heterogeneous and homogeneous metal catalysis.
The surface modification of metal nanocatalysts with organometallic
motifs provides a new design principle of metal catalysts with enhanced
catalysis.
The first 60 cases constitute the early stage of the learning curve for endoscopic thyroidectomy. The proficiency and stability of the operation reach the advanced level after 150 cases.
A mesoporous nickel layer is used as the counter electrode in printable perovskite solar cells. A unique reuse process is realized in such perovskite solar cell devices by repeated loading of the perovskite material. Under standard AM1.5 illumination, the fresh device shows a promising power conversion efficiency of 13.6%, and an efficiency of 12.1% is obtained in the reused devices.
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