Significance The combined radical and nonradical reactions induced by peroxymonosulfate (PMS) activation can promise deep mineralization and selective removal of micropollutants from complex wastewater. However, nonhomogeneous metal-based catalysts with single active sites lead to a low efficiency of electron cycling for both radical and nonradical generation. In this study, asymmetric Co–O–Bi sites were constructed to achieve rapid electron cycling while achieving site synergy, thus effectively activating PMS to generate radicals and nonradicals. The presence of asymmetric sites can tune and optimize the catalytic performance through structural modulation, which can effectively remove and mineralize micropollutants from organic and inorganic compounds under the environmental background.

Generating dual-active species by triple-atom sites through peroxymonosulfate activation for treating micropollutants in complex water

Rare-earth (RE)-based transition metal oxides (TMO) are emerging as a frontier towards oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. Herein, we successfully design and synthesize atomically dispersed Ce on CoO by an effective plasma (P)-assisted strategy as a model (P-Ce SAs@CoO) to investigate the origin of OER performance in RE-TMO systems. The P-Ce SAs@CoO exhibits favorable performance with an overpotential of only 261 mV at 10 mA cm-2 and robust electrochemical stability, superior to individual CoO. X-ray absorption spectroscopy and in-situ electrochemical Raman spectroscopy uncover that the Ce-induced electron redistribution inhibits Co-O bond breakage in the Co-O-Ce unit site. Theoretical analyses demonstrate that the gradient orbital coupling reinforces the Co-O covalency of Ce(4f)-O(2p)-Co(3d) unit active site with an optimized Co-3d-eg occupancy, which can balance the adsorption strength of intermediates and in turn reach the apex of the theoretical OER maximum, in excellent agreement with experimental observations. We believe the establishment of this Ce-CoO model can set a basis for the mechanistic understanding and structural design of high-performance RE-TMO catalysts. This article is protected by copyright. All rights reserved.

Reinforce the Co-O Covalency via Ce(4f)-O(2p)-Co(3d) Gradient Orbital Coupling for High-efficiency Oxygen Evolution.

Electrocatalytic water splitting driven by renewable electricity has been recognized as a promising approach for green hydrogen production. Different from conventional strategies in developing electrocatalysts for the two half-reactions of water splitting (e.g., the hydrogen and oxygen evolution reactions, HER and OER) separately, there has been a growing interest in designing and developing bifunctional electrocatalysts, which are able to catalyze both the HER and OER. In addition, considering the high overpotentials required for OER while limited value of the produced oxygen, there is another rapidly growing interest in exploring alternative oxidation reactions to replace OER for hybrid water splitting toward energy-efficient hydrogen generation. This Review begins with an introduction on the fundamental aspects of water splitting, followed by a thorough discussion on various physicochemical characterization techniques that are frequently employed in probing the active sites, with an emphasis on the reconstruction of bifunctional electrocatalysts during redox electrolysis. The design, synthesis, and performance of diverse bifunctional electrocatalysts based on noble metals, nonprecious metals, and metal-free nanocarbons, for overall water splitting in acidic and alkaline electrolytes, are thoroughly summarized and compared. Next, their application toward hybrid water splitting is also presented, wherein the alternative anodic reactions include sacrificing agents oxidation, pollutants oxidative degradation, and organics oxidative upgrading. Finally, a concise statement on the current challenges and future opportunities of bifunctional electrocatalysts for both overall and hybrid water splitting is presented in the hope of guiding future endeavors in the quest for energy-efficient and sustainable green hydrogen production.

Bifunctional Electrocatalysts for Overall and Hybrid Water Splitting.

Polymer electrolyte membrane water electrolysis (PEMWE) has been regarded as a promising technology for renewable hydrogen production. However, acidic oxygen evolution reaction (OER) catalysts with long-term stability impose a grand challenge in its large-scale industrialization. In this review, critical factors that may lead to catalyst's instability in couple with potential solutions are comprehensively discussed, including mechanical peeling, substrate corrosion, active-site over-oxidation/dissolution, reconstruction, oxide crystal structure collapse through the lattice oxygen-participated reaction pathway, etc. Last but not least, personal prospects are provided in terms of rigorous stability evaluation criteria, in situ/operando characterizations, economic feasibility and practical electrolyzer consideration, highlighting the ternary relationship of structure evolution, industrial-relevant activity and stability to serve as a roadmap towards the ultimate application of PEMWE. 

Long‐Term Stability Challenges and Opportunities in Acidic Oxygen Evolution Electrocatalysis

Polymer electrolyte membrane water electrolysis (PEMWE) has been regarded as a promising technology for renewable hydrogen production. However, acidic oxygen evolution reaction (OER) catalysts with long-term stability imposes a grand challenge in its large-scale industrialization. In this review, critical factors that may lead to catalyst's instability in couple with potential solutions are comprehensively discussed, including mechanical peeling, substrate corrosion, active-site over-oxidation/dissolution, reconstruction, oxide crystal structure collapse through the lattice oxygen-participated reaction pathway, etc. Last but not least, personal prospects are provided in terms of rigorous stability evaluation criteria, in situ/operando characterizations, economic feasibility and practical electrolyzer consideration, highlighting the ternary relationship of structure evolution, industrial-relevant activity and stability to serve as a roadmap towards the ultimate application of PEMWE.

Long-Term Stability Challenges and Opportunities in Acidic Oxygen Evolution Electrocatalysis.

Developing non-noble catalysts with superior activity and durability for oxygen evolution reaction (OER) in acidic media is paramount for hydrogen production from water. Still, challenges remain due to the inadequate activity and stability of the OER catalyst. Here, we report a cost-effective and stable manganese oxybromide (Mn7.5O10Br3) catalyst exhibiting an excellent OER activity in acidic electrolytes, with an overpotential of as low as 295 ± 5 mV at a current density of 10 mA cm-2. Mn7.5O10Br3 maintains good stability under operating conditions for at least 500 h. In situ Raman spectroscopy, X ray absorption near edge spectroscopy, and density functional theory calculations confirm that a self-oxidized surface with enhanced electronic transmission capacity forms on Mn7.5O10Br3 and is responsible for both the high catalytic activity and long-term stability during catalysis. The development of Mn7.5O10Br3 as an OER catalyst provides crucial insights into the design of non-noble metal electrocatalysts for water oxidation. 

/pdf/efficient-and-stable-noble-metal-free-catalyst-for-acidic-1ocsh18i.pdf

Efficient and stable noble-metal-free catalyst for acidic water oxidation

The effect of microwave coupled hot air drying on rehydration ratio (RR) and total sugar content (TSC) of Chinese yam was investigated. Single factor test and response surface methodology were used for process parameter optimization with hot air temperature, hot air velocity, slice thickness, and microwave power density as variables and RR and TSC of dried products as responses. The effect of variables on RR followed the order: slice thickness > hot air temperature > microwave power density > hot air velocity. The effect of variables on TSC followed the order: slice thickness > microwave power density > hot air velocity > hot air temperature. The optimized process parameters were hot air velocity of 2.5 m/s, hot air temperature of 61.7 °C, slice thickness of 8.5 mm, and microwave power density of 5.9 W/g. Under the optimal conditions, the predicted values of RR and TSC were 1.90 g/g and 5.74 g/100 g, respectively, which is very close to corresponding actual values (1.83 g/g and 5.72 g/100 g). The desirability of 0.913 further validated the effectiveness of the model. The findings from this work may apply to other agricultural products.

https://www.mdpi.com/2227-9717/7/10/745/pdf

Optimization of Microwave Coupled Hot Air Drying for Chinese Yam Using Response Surface Methodology

Hot-air coupled microwave was employed to dry lotus root slices. The effects of lotus root slice thickness (5, 8, 11, 14, and 17 mm), hot-air velocity (1.5, 2.0, 2.5, 3.0, and 3.5 m/s), hot-air temperature (50, 55, 60, 65, and 70 °C), and microwave power density (2, 4, 6, 8, and 10 W/g) on drying characteristics and kinetics were studied. Results indicated that the drying process involved both the accelerating and decelerating periods but no constant rate period. The drying rate reached the maximum of 1.52 kg/kg when microwave power density was 8 W/g and reached the minimum of 0.02 kg/kg at the last stage of drying. In addition, the drying kinetics of lotus root slices were also investigated using eleven previously reported models. Among the models, the Verma et al. model was the most suitable for description of the drying behaviors of lotus root slices based on R 2, root-mean-square error, and chi-square. The moisture transfer from lotus root slices can be effectively described by Fick's diffusion model. Regardless of drying conditions, the effective diffusivity coefficients ranged from 8.23 × 10-7 to 7.08 × 10-6 m2/s, and their variations were mostly in agreement with those of moisture ratios. The activation energy of moisture diffusion related to lotus root slices was determined to be 13.754 kJ/mol.

Effects of Hot-Air Coupled Microwave on Characteristics and Kinetics Drying of Lotus Root Slices.

A study on the association between biomass types and magnesium oxide pretreatment.

Boosting fermentable sugars by integrating magnesium oxide-treated corn stover and corn stover liquor without washing and detoxification.

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