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Eco-utilization of silicon-rich lye: Synthesis of amorphous calcium silicate hydrate and its application for recovering heavy metals
No full textDuring sustainable high-value utilization of coal-based solid wastes, a kind of characteristic silicon-rich lye (SRL) generated, and its comprehensive recovery and recycling remains an important subject. Through a simple and facile strategy of mild caustic-crystallization method, SRL was favorably utilized through calcium silicate hydrate (C-S-H) synthesis with silicon conversion efficiency over 97.33%. The micro-morphology of C-S-H presented a typical "honeybee hive " like porous structure with numerous exchangeable activity cations and combination sites in the silicate chain structure. The amorphous C-S-H products possessed marvelous recovery abilities for typical heavy metals as Cu (II), Zn (II), and Cr (III) in industrial wastewater with recovery efficiency all above 99.6% in quite a short period. The recovery mechanism of C-S-H toward heavy metals was revealed as calcium ions exchange and interlayer structure combination with SiO4 and AlO4 tetrahedron through the analysis of characterization technologies and DFT simulation calculation. C-S-H synthesized in SRL contributes to achieving valuable resources conversion and recycling for guiding sustainable development of coal-based solid waste comprehensive utilization
Youth Innovation Promotion Association of the Chinese Academy of Sciences of China[2018064]
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Xiangyuan County Solid Waste Comprehensive Utilization Science and Technology Project[2018XYSDYY-10]
No full textKorea Institute of Energy Technology Evaluation and Planning (KETEP) grant - Ministry of Trade, Industry and Energy of the Republic of Korea (MOTIE)[20202020800330]
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<p>Nitrogen-doped carbon black supported synergistic palladium single atoms and nanoparticles for electrocatalytic oxidation of methanol</p>
No full textFor commercially viable direct methanol fuel cells, electrocatalysts play a crucial role in motivating the sluggish methanol oxidation reaction (MOR) over anode. Unfortunately, the large-scale applications of current MOR catalysts are hampered by their poor tolerance to poisoning and fast activity degradation. Herein, a unique composite catalyst comprised of partial Pd nanoparticles and partial Pd single atoms (Pd-NPs/Pd-N-x@C) is developed. The as-fabricated catalyst exhibits remarkable activity of 9.45 mA.cm(-2) towards MOR in alkaline solution, which is 7.05 and 3.92 times that of commercial Pd/C and nanoparticle type (Pd-NPs@C) electro-catalysts, respectively. Impressively, the Pd-NPs/Pd-N-x@C shows the highest long-time stability with 90.38% and 89.8% of the initial activity retained after 3600 s chronoamperometry (CA) test and 2000 cycles of cyclic voltammetry (CV) measurements with accelerated durability test (ADT), respectively. Combined with high-angle annular darkfield scanning transmission electron microscopy (HAADF-STEM), X-ray adsorption fine structure (XAFS) spectra and X-ray photoelectron spectroscopy (XPS) analyses, the superior performance of Pd-NPs/Pd-N-x@C can be ascribed to the synergistic effect from the Pd single atoms, N-doped carbon supports and Pd nanoparticles. Notably, the embedded Pd single atoms are liable to transfer electrons to the substrate due to the electronic metal-support interactions (EMSI) and the charge transfer between Pd nanoparticles and carbon supports is suppressed, inducing a weak adsorption strength of poisonous carbonous intermediate species on active Pd nanoparticles and improved poisoning tolerance in MOR process, which is verified by density functional theory (DFT) calculations as well as CO-stripping voltammetry experiments. This work not only con-tributes the first example of a synergistic catalyst between nanoparticles and single atoms for MOR but also deepens the knowledge on the metal-support interaction
