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22 records · Page 2

Hierarchically structured MoO 2 /dopamine-derived carbon spheres as intercalation electrodes for lithium-ion batteries

A hydrogen peroxide initiated sol-gel process involving molybdenum transformation in the presence of dopamine (Dopa) hydrochloride excess produced the metastable precipitate composed of polydopamine (PDopa) spheres coated with Dopa preintercalated molybdenum oxide, (Dopa) x MoO y @PDopa. The hydrothermal treatment (HT) of the (Dopa) x MoO y @PDopa precursor resulted in the simultaneous carbonization of Dopa and molybdenum reduction generating MoO 2 nanoplatelets distributed and confined on the surface of the Dopa-derived carbon matrix (HT-MoO 2 /C). The consecutive annealing (An) of the HT-MoO 2 /C sample at 600 °C under Ar atmosphere led to the formation of MoO 2 with increased Mo oxidation state and improved structural stability (AnHT-MoO 2 /C). Annealing had also further facilitated interaction between the molybdenum-derived and Dopa-derived components resulting in the modification of the carbon matrix confirmed by Raman spectroscopy. Morphology of both materials is best described as Dopa-derived carbon spheres decorated with MoO 2 nanoplatelets. These integrated metal oxide and carbon structures were tested as electrodes for lithium-ion batteries in the potential window that corresponds to the intercalation mechanism of charge storage. The AnHT-MoO 2 /C electrode showed enhanced electrochemical activity, with an initial specific discharge capacity of 260 mAh/g and capacity retention of 67% after 50 cycles, compared to the HT-MoO 2 /C electrode which exhibited an initial specific discharge capacity of 235 mAh g –1 and capacity retention of 47% after 50 cycles. The rate capability experiments revealed that the capacity of 93 mAh/g and 120 mAh/g was delivered by the HT-MoO 2 /C and AnHT-MoO 2 /C electrodes, respectively, when the current density was increased to 100 mA/g. Here, the improved specific capacity, electrochemical stability, and rate capability achieved after annealing were attributed to higher crystallinity of MoO 2 , increased oxidation state of Mo, and formation of the tighter MoO 2 /carbon contact accompanied by the annealing assisted interaction between MoO 2 and Dopa-derived carbon.

25 ENERGY STORAGE↗

Synergistic Solvent-Surface Interactions Enable Alkyne Semihydrogenation at Palladium

Enabling higher yield and better selectivity for fine-chemical synthesis through heterogeneous catalysis is intricately linked to the interplay of active sites, reaction conditions, and mass transfer influence provided by the catalyst. Alkyne semihydrogenation is ubiquitous in the production of bulk chemicals in the pharmaceutical, polymer, or fine-chemical industries, but product selectivity remains a major challenge. Here, in this study, we demonstrate that the design of catalysts encompassing nickel (Ni) foams as contiguous monolith supports, decorated with ultralow loading of Pd/PdO x nanoparticles on a carbonized polydopamine interface and tuned with a thin layer of Al 2 O 3 , in conjunction with an optimized reaction environment leads to highly selective alkyne semihydrogenation. The reactions demonstrate good functional group tolerance and applicability to flow reactor systems. Combined computational and experimental studies are presented to describe the synergistic effect between the solvent-surface interaction and the degree of Pd surface reduction that are necessary to promote this selectivity. The system highlights the opportunity for catalyst-solvent codesign as a benign alternative to more complex reactants featuring extrinsic poisons or less-favored dopants.

atomic layer deposition↗

Probing sub-5 Ångstrom micropores in carbon for precise light olefin/paraffin separation

Olefin/paraffin separation is an important but challenging and energy-intensive process in petrochemical industry. The realization of carbons with size-exclusion capability is highly desirable but rarely reported. Herein, we report polydopamine-derived carbons (PDA-Cx, where x refers to the pyrolysis temperature) with tailorable sub-5 Å micropore orifices together with larger microvoids by one-step pyrolysis. The sub-5 Å micropore orifices centered at 4.1–4.3 Å in PDA-C800 and 3.7–4.0 Å in PDA-C900 allow the entry of olefins while entirely excluding their paraffin counterparts, performing a precise cut-off to discriminate olefin/paraffin with sub-angstrom discrepancy. The larger voids enable high C 2 H 4 and C 3 H 6 capacities of 2.25 and 1.98 mmol g –1 under ambient conditions, respectively. Breakthrough experiments confirm that a one-step adsorption-desorption process can obtain high-purity olefins. Inelastic neutron scattering further reveals the host–guest interaction of adsorbed C 2 H 4 and C 3 H 6 molecules in PDA-Cx. This study opens an avenue to exploit the sub-5 Å micropores in carbon and their desirable size-exclusion effect.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Suspended Membrane Evaporators Integrating Environmental and Solar Evaporation for Oily Wastewater Purification

Solar-driven evaporation is promising in oily wastewater treatment, in particular for emulsions, but conventional evaporators suffer from pore blocking by residual oil or contamination by volatile oil compounds in the condensed water. In the current research, we develop a suspended membrane evaporator integrating solar evaporation with oil-in-water emulsion separation. The heating and evaporating interface is separated from the rejecting interface to avoid oil escape and improve heat management. A temperature gradient forms on the membrane surface that can promote evaporation performance by combining both solar and environmental evaporation. Such an evaporator achieves a maximum evaporation rate of 1.645 kg/(m 2 ·h) as well as an apparent evaporation efficiency of 111.9%. Moreover, the superhydrophilic and superoleophobic membrane shows excellent oil repellence and emulsion rejection, which can achieve an oil removal efficiency above 98.8% in oil-in-water emulsion separation, and high evaporation rate recovery in cycling tests. Furthermore, a scaled-up membrane evaporator array produces ~8 kg/(m 2 ·d) of clean water from oily wastewater in outdoor experiments, further demonstrating the strong purification performance of this evaporator in oily wastewater treatment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗