Diffusion is an extremely critical step in zeolite catalysis which determines the catalytic performance, in particular for the conversion of bulky molecules. Introducing interconnected mesopores and macropores into a single microporous zeolite with the rationalized pore size at each level is an effective strategy to suppress the diffusion limitations, but remains highly challenging due to the lack of rational design principles. Herein, we demonstrate the first example of boosting molecular diffusion by constructing hierarchical Murray zeolites with highly ordered and fully interconnected macro-meso-microporous structure on the basis of the generalized Murray's Law. Such hierarchical Murray zeolite with a refined quantitative relationship between pore size at each length scale exhibited 9 and 5 times higher effective diffusion rate, leading to 2.5 and 1.5 times higher catalytic performance in the bulky 1,3,5-triisopropylbenzene cracking reaction than those of microporous ZSM-5 and ZSM-5 nanocrystals, respectively. The concept of hierarchical Murray zeolites with optimized structural feature and their design principles could be applied to other catalytic reactions for maximized performance.
The development of metal-halide perovskite nanocrystals (NCs) that yield bright and stable emission is of great importance. Previous reported perovskite NCs are mostly based on APbX 3 -type family fabricated via ligand-or surfactant-assisted chemical approaches. However, realizing bright and stable emission remains a challenge because of desorption of ligands/surfactants during long-term operation. Herein, Ruddlesden-Popper (RP)-type (A) 2 (MA) n-1 Pb n Br 3n+1 NCs with size less than Bohr radius stabilized in mesoporous silica scaffold, which are prepared in situ via physical approach at low temperature are introduced. The RP NCs in mesoporous silica exhibit the formation of spatially and electronically separated quantum wells, efficient energy funneling between different n phases for bright emission (photoluminescence quantum yields of ≈99%), high irradiation stability (T 70 = 110 days), and long-term stability (T 90 = 110 days).These RP NCs have broad potential for bright light-emitting diodes, highresolution PL imaging, and waterproof inks. Importantly, for the first time, stretchable perovskite X-ray scintillator is demon strated with excellent X-ray imaging with resolution greater than 14 line pairs mm -1 . These findings offer a paradigm to motivate future research toward stable and efficient perovskite optoelectronics.
Guided
by the theoretical calculation, achieving an efficient hydrogen
evolution reaction (HER) by S-vacancy engineering toward MoS2-based materials is quite challenging due to the contradictory relationship
between the adsorption free energy of hydrogen atoms (ΔG
H) of the exposed Mo atoms (EMAs) and the number
of EMAs per unit area (N
EMAs). Herein,
we demonstrate a novel one-pot incorporating-assisted compositing
strategy to realize fine-tuning the concentration of S-vacancies (C
S‑vacancies) of MoS2-based
materials to boost highly active EMAs for efficient HER. In our strategy,
S-vacancies are modulated into basal planes of MoS2
via decreasing the formation energy of S-vacancies by oxygen
incorporation; moreover, C
S‑vacancies of the basal planes is precisely regulated by simply controlling
the molar amount of the Co precursor based on the electron injection
effect. At low or excessively high C
S‑vacancies, the as-synthesized electrocatalysts lack “highly active
EMAs” in quantity or nature. The balance between the intrinsic
activity of EMAs and N
EMAs is realized
for boosting EMAs with high catalytic performance. The optimal electrocatalysts
exhibit excellent activity and stability at fine-tuning C
S‑vacancies to 9.61%. Our results will pave a novel
strategy for unlocking the potential of an inert basal plane in MoS2 for high-performance HER.
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