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Methanogens play an important role in the demethylation of arsenic. Soil amendments that inhibit methanogens can increase dimethylarsinic acid (DMA), which is responsible for straighthead disease in rice. A decrease in methanogenesis caused by silicate fertilizer may increase DMA concentration in paddy soils and rice grains; the relationship between these two factors and their impacts on DMA concentration remains unclear. We applied silicate fertilizer (2 Mg ha -1 ) to japonica and indica rice grown on arsenic-spiked soils and found a simultaneous reduction in methane emissions and pore-water DMA concentration, compared to no-silicate fertilization. Gene and transcript copies of mcrA and arsM, as well as dominant methanogens and arsenic-methylating microbes decreased significantly with silicate fertilization. However, the sulfate-reducing bacteria and the gene and transcript copies of dsrB did not change significantly in response to the application of silicate fertilizer to paddy soils. The abundance of arsenic methylating microbes was significantly and positively correlated with the abundance of methanogens, but not with the abundance of sulfate-reducing bacteria. Methylomonas and Methylobacter, which harbor the arsM gene, were suppressed under silicate fertilization, suggesting that they have the potential to methylate As and play a crucial role in reducing pore-water DMA in As-enriched flooded paddy soils. Increasing Fe concentration, soil pH, and Eh value decreased pore-water DMA concentration, while decreasing arsenite concentration, arsM and mcrA gene abundance decreased it. While silicate fertilization decreased arsenite and DMA concentrations in pore-water, it had no significant effect on rice DMA content, but significantly decreased arsenite content. Results reveal that methanogens and arsenic-methylating microbes have a synergistic relationship under silicate fertilization that facilitates a significant reduction in methane emissions and DMA concentration in As-enriched paddy soils., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

Redox chemistry involving the quinone/phenol cycling of natural organic matter (NOM) is known to modulate microbial respiration. Complexation with metals or minerals can also affect NOM solubilization and stability. Inspired by these natural phenomena, a new soil amendment approach was suggested to effectively decrease methane emissions in flooded rice paddies. Structurally stable forms of NOM such as lignin and humic acids (HAs) were shown to decrease methane gas emissions in a vial experiment using different soil types and rice straw as a methanogenic substrate, and this inhibitory behavior was likely enhanced by ferric ion-NOM complexation. A mechanistic study using HAs revealed that complexation facilitated the slow release of the humic components. Interestingly, borohydride-based reduction, which transformed quinone moieties into phenols, caused the HAs to lose their inhibitory capacity, suggesting that the electron-accepting ability of HAs is vital for their inhibitory effect. In rice field tests, the humic-metal complexes were shown to successfully mitigate methane generation, while carbon dioxide emissions were relatively unchanged. Microbial community analysis of the rice fields by season revealed a decrease in specific cellulose-metabolizing and methanogenic genera associated with methane emissions. In contrast, the relative abundance of Thaumarchaeota and Actinomycetota, which are associated with NOM and recalcitrant organics, was higher in the presence of Fe-stabilized HAs. These microbial dynamics suggest that the slow release of humic components is effective in modulating the anoxic soil microbiome, possibly due to their electron-accepting ability. Given the simplicity, cost-effectiveness, and soil-friendly nature of complexation processes, Fe-stabilized NOM represents a promising approach for the mitigation of methane emissions from flooded rice paddies., Competing Interests: Declaration of competing interest The authors declare no competing financial interest., (Copyright © 2024. Published by Elsevier B.V.)