Recent progress in energy-saving electrocatalytic hydrogen production via regulating the anodic oxidation reaction.

Hydrogen energy with its advantages of high calorific value, renewable nature, and zero carbon emissions is considered an ideal candidate for clean energy in the future. The electrochemical decomposition of water, powered by renewable and clean energy sources, presents a sustainable and environmentally friendly approach to hydrogen production. However, the traditional electrochemical overall water-splitting reaction (OWSR) is limited by the anodic oxygen evolution reaction (OER) with sluggish kinetics. Although important advances have been made in efficient OER catalysts, the theoretical thermodynamic difficulty predetermines the inevitable large potential (1.23 V vs. RHE for the OER) and high energy consumption for the conventional water electrolysis to obtain H2. Besides, the generation of reactive oxygen species at high oxidation potentials can lead to equipment degradation and increase maintenance costs. Therefore, to address these challenges, thermodynamically favorable anodic oxidation reactions with lower oxidation potentials than the OER are used to couple with the cathodic hydrogen evolution reaction (HER) to construct new coupling hydrogen production systems. Meanwhile, a series of robust catalysts applied in these new coupled systems are exploited to improve the energy conversion efficiency of hydrogen production. Besides, the electrochemical neutralization energy (ENE) of the asymmetric electrolytes with a pH gradient can further promote the decrease in application voltage and energy consumption for hydrogen production. In this review, we aim to provide an overview of the advancements in electrochemical hydrogen production strategies with low energy consumption, including (1) the traditional electrochemical overall water splitting reaction (OWSR, HER-OER); (2) the small molecule sacrificial agent oxidation reaction (SAOR) and (3) the electrochemical oxidation synthesis reaction (EOSR) coupling with the HER (HER-SAOR, HER-EOSR), respectively; (4) regulating the pH gradient of the cathodic and anodic electrolytes. The operating principle, advantages, and the latest progress of these hydrogen production systems are analyzed in detail. In particular, the recent progress in the catalytic materials applied to these coupled systems and the corresponding catalytic mechanism are further discussed. Furthermore, we also provide a perspective on the potential challenges and future directions to foster advancements in electrocatalytic green sustainable hydrogen production.

Regulating the thickness of the carbon coating layer in iron/carbon heterostructures to enhance the catalytic performance for oxygen evolution reaction.

The exploration of high-performance electrocatalysts for the oxygen evolution reaction (OER) is crucial and urgent for the fast development of green and renewable hydrogen energy. Herein, an ultra-fast and energy-efficient preparation strategy (microwave-assisted rapid in-situ pyrolysis of organometallic compounds induced by carbon nanotube (CNT)) is developed to obtain iron/carbon (Fe/C) heterogeneous materials (Fe/Fe3C particles wrapped by carbon coating layer). The thickness of the carbon coating layer can be adjusted by changing the content and form of carbon in the metal sources during the fast preparation process. Fe/Fe3C-A@CNT using iron acetylacetonate as metal sources possesses unique Fe/C heterogeneous, small Fe/Fe3C particles encapsulated by the thin carbon coating layer (1.77 nm), and obtains the optimal electron penetration effect. The electron penetration effect derives from the redistribution of charge between the surface carbon coating layer and inner Fe/Fe3C nanoparticles efficiently improving both catalytic activity and stability. Therefore, Fe/Fe3C-A@CNT shows efficient OER catalytic activity, just needing a low overpotential of 292 mV to reach a current density of 10 mA cm-2, and long-lasting stability. More importantly, the unique control strategy for carbon thickness in this work provides more opportunity and perspective to prepare robust metal/carbon-based catalytic materials at the nanoscale.

Utilizing the cross-linked effect and reconstruction strategy of phytic acid to build Fe-Co-Ni trimetallic amorphous carbon-matrix compounds as efficient oxygen evolution catalyst.

Developing low-cost electrocatalysts with excellent activity is significant for accelerating the slow oxygen evolution reaction (OER). In this work, an effective electrocatalyst is prepared via the cross-linked effect and reconstruction strategy based on inexpensive transition metals (Fe, Co, and Ni) and phytic acid (PA). The feasibility of utilizing the cross-linked effect and reconstruction strategy is due to that PA molecules with strongly electronegative phosphoric acid groups possess a great deal of complexing sites, which can facilitate the formation of large cross-linked network by randomly complexing Fe, Co and Ni ions. And the carboatomic rings in PA molecules will reconstructed as carbon-matrix when PA molecules decompose. The above structural evolution of large cross-linked network and reconstructing process is rigorously analyzed through the characterization methods such as XPS. These analysis results indicate that FeCoNi-PA-300 possesses a high degree of amorphization, an abundant nanoporous structure, and a small nanoparticle size, resulting in a large electrochemically active area. Consequently, FeCoNi-PA-300 just needs low overpotentials of about 271 mV and 286 mV to obtain the current densities of 50 and 100 mA cm-2, respectively. Meaningfully, this synthetic method is a general strategy to meliorate the OER activity and electrical conductivity of other catalysts.

Determination of the MiRNAs Related to Bean Pyralid Larvae Resistance in Soybean Using Small RNA and Transcriptome Sequencing.

Soybean is one of the most important oil crops in the world. Bean pyralid is a major leaf-feeding insect of soybean. In order to screen out the functional genes and regulatory pathways related to the resistance for bean pyralid larvae, the small RNA and transcriptome sequencing were performed based on the highly resistant material (Gantai-2-2) and highly susceptible material (Wan 82-178) of soybean. The results showed that, when comparing 48 h feeding with 0 h feeding, 55 differentially expressed miRNAs were identified in Gantai-2-2 and 58 differentially expressed miRNAs were identified in Wan82-178. When comparing Gantai-2-2 with Wan82-178, 77 differentially expressed miRNAs were identified at 0 h feeding, and 70 differentially expressed miRNAs were identified at 48 h feeding. The pathway analysis of the predicted target genes revealed that the plant hormone signal transduction, RNA transport, protein processing in the endoplasmic reticulum, zeatin biosynthesis, ubiquinone and other terpenoid-quinone biosynthesis, and isoquinoline alkaloid biosynthesis may play important roles in soybean's defense against the stress caused by bean pyralid larvae. According to conjoint analysis of the miRNA/mRNA, a total of 20 differentially expressed miRNAs were negatively correlated with 26 differentially expressed target genes. The qRT-PCR analysis verified that the small RNA sequencing results were credible. According to the analyses of the differentially expressed miRNAs, we speculated that miRNAs are more likely to play key roles in the resistance to insects. Gma-miR156q, Gma-miR166u, Gma-miR166b, Gma-miR166j-3p, Gma-miR319d, Gma-miR394a-3p, Gma-miR396e, and so on-as well as their negatively regulated differentially expressed target genes-may be involved in the regulation of soybean resistance to bean pyralid larvae. These results laid a foundation for further in-depth research regarding the action mechanisms of insect resistance.

Comparative transcriptome analysis of soybean response to bean pyralid larvae.

BACKGROUND: Soybean is one of most important oilseed crop worldwide, however, its production is often limited by many insect pests. Bean pyralid is one of the major soybean leaf-feeding insects in China. To explore the defense mechanisms of soybean resistance to bean pyralid, the comparative transcriptome sequencing was completed between the leaves infested with bean pyralid larvae and no worm of soybean (Gantai-2-2 and Wan82-178) on the Illumina HiSeq™ 2000 platform. RESULTS: In total, we identified 1744 differentially expressed genes (DEGs) in the leaves of Gantai-2-2 (1064) and Wan82-178 (680) fed by bean pyralid for 48 h, compared to 0 h. Interestingly, 315 DEGs were shared by Gantai-2-2 and Wan82-178, while 749 and 365 DEGs specifically identified in Gantai-2-2 and Wan82-178, respectively. When comparing Gantai-2-2 with Wan82-178, 605 DEGs were identified at 0 h feeding, and 468 DEGs were identified at 48 h feeding. Gene Ontology (GO) annotation analysis revealed that the DEGs were mainly involved in the metabolic process, single-organism process, cellular process, responses to stimulus, catalytic activities and binding. Pathway analysis showed that most of the DEGs were associated with the plant-pathogen interaction, phenylpropanoid biosynthesis, phenylalanine metabolism, flavonoid biosynthesis, peroxisome, plant hormone signal transduction, terpenoid backbone biosynthesis, and so on. Finally, we used qRT-PCR to validate the expression patterns of several genes and the results showed an excellent agreement with deep sequencing. CONCLUSIONS: According to the comparative transcriptome analysis results and related literature reports, we concluded that the response to bean pyralid feeding might be related to the disturbed functions and metabolism pathways of some key DEGs, such as DEGs involved in the ROS removal system, plant hormone metabolism, intracellular signal transduction pathways, secondary metabolism, transcription factors, biotic and abiotic stresses. We speculated that these genes may have played an important role in synthesizing substances to resist insect attacks in soybean. Our results provide a valuable resource of soybean defense genes that will benefit other studies in this field.

Proteomic analysis by iTRAQ-MRM of soybean resistance to Lamprosema Indicate.

BACKGROUND: Lamprosema indicate is a major leaf feeding insect pest to soybean, which has caused serious yield losses in central and southern China. To explore the defense mechanisms of soybean resistance to Lamprosema indicate, a highly resistant line (Gantai-2-2) and a highly susceptible line (Wan 82-178) were exposed to Lamprosema indicate larval feedings for 0 h and 48 h, and the differential proteomic analyses of these two lines were carried out. RESULTS: The results showed that 31 differentially expressed proteins (DEPs) were identified in the Gantai-2-2 when comparing 48 h feeding with 0 h feeding, and 53 DEPs were identified in the Wan 82-178. 28 DEPs were identified when comparing Gantai-2-2 with Wan 82-178 at 0 h feeding. The bioinformatic analysis results showed that most of the DEPs were associated with ribosome, linoleic acid metabolism, flavonoid biosynthesis, phenylpropanoid biosynthesis, peroxisome, stilbenoid, diarylheptanoid and gingerol biosynthesis, glutathione metabolism, pant hormone signal transduction, and flavone and flavonol biosynthesis, as well as other resistance related metabolic pathways. The MRM analysis showed that the iTRAQ results were reliable. CONCLUSIONS: According to the analysis of the DEPs results, the soybean defended or resisted the Lamprosema indicate damage by the induction of a synthesis of anti-digestive proteins which inhibit the growth and development of insects, reactive oxygen species scavenging, signaling pathways, secondary metabolites synthesis, and so on.