Microenvironment drives cell state, plasticity, and drug response in pancreatic cancer.

Prognostically relevant RNA expression states exist in pancreatic ductal adenocarcinoma (PDAC), but our understanding of their drivers, stability, and relationship to therapeutic response is limited. To examine these attributes systematically, we profiled metastatic biopsies and matched organoid models at single-cell resolution. In vivo, we identify a new intermediate PDAC transcriptional cell state and uncover distinct site- and state-specific tumor microenvironments (TMEs). Benchmarking models against this reference map, we reveal strong culture-specific biases in cancer cell transcriptional state representation driven by altered TME signals. We restore expression state heterogeneity by adding back in vivo-relevant factors and show plasticity in culture models. Further, we prove that non-genetic modulation of cell state can strongly influence drug responses, uncovering state-specific vulnerabilities. This work provides a broadly applicable framework for aligning cell states across in vivo and ex vivo settings, identifying drivers of transcriptional plasticity and manipulating cell state to target associated vulnerabilities.

High-Resolution Estimates of N2O Emissions from Inland Waters and Wetlands in China.

Inland waters (rivers, lakes, and reservoirs) and wetlands (marshes and coastal wetlands) represent large and continuous sources of nitrous oxide (N2O) emissions, in view of adequate biomass and anaerobic conditions. Considerable uncertainties remain in quantifying spatially explicit N2O emissions from aquatic systems, attributable to the limitations of models and a lack of comprehensive data sets. Herein, we conducted a synthesis of 1659 observations of N2O emission rates to determine the major environmental drivers across five aquatic systems. A framework for spatially explicit estimates of N2O emissions in China was established, employing a data-driven approach that upscaled from site-specific N2O fluxes to robust multiple-regression models. Results revealed the effectiveness of models incorporating soil organic carbon and water content for marshes and coastal wetlands, as well as water nitrate concentration and dissolved organic carbon for lakes, rivers, and reservoirs for predicting emissions. Total national N2O emissions from inland waters and wetlands were 1.02 × 105 t N2O yr-1, with contributions from marshes (36.33%), rivers (27.77%), lakes (25.27%), reservoirs (6.47%), and coastal wetlands (4.16%). Spatially, larger emissions occurred in the Songliao River Basin and Continental River Basin, primarily due to their substantial terrestrial biomass. This study offers a vital national inventory of N2O emissions from inland waters and wetlands in China, providing paradigms for the inventorying work in other countries and insights to formulate effective mitigation strategies for climate change.

Correlation Study on the Prognostic Value of miR-21 and S-100B Protein Levels in Neonatal Hypoxic-Ischemic Encephalopathy Undergoing Hypothermia Therapy.

OBJECTIVE: To evaluate the variations in serum levels of microRNA-21 (miR-21) and S-100B protein in neonates with hypoxic-ischemic encephalopathy (HIE) after receiving hypothermia therapy and explore the correlation of these biomarkers with the neurodevelopmental prognosis of the infants. METHODS: This retrospective analysis included 90 neonatal HIE patients diagnosed and treated between January 2019 and December 2022. Real-time quantitative PCR and enzyme-linked immunosorbent assay (ELISA) methods were used to measure miR-21 and S-100B protein levels. Neurodevelopmental assessments were conducted at one year, and follow-up was performed using the Bayley Scales of Infant and Toddler Development third edition. Statistical analysis was carried out using SPSS software, with t-tests for continuous variables, chi-square tests for categorical data, Pearson correlation coefficient for correlation analysis, and multivariate regression analysis to adjust for confounding factors. RESULTS: After hypothermia therapy, the observation group showed a significant decrease in miR-21 and S-100B protein levels (P < 0.001), and neurodevelopmental scores were significantly higher than the control group (P < 0.05). Correlation analysis indicated a negative correlation between miR-21 and neurodevelopmental scores (r=-0.62, P < 0.001), as well as a negative correlation between S-100B protein levels (r=-0.76, P < 0.001). Multivariate regression analysis demonstrated that miR-21 levels and S-100B protein levels maintained independent negative correlations with neurodevelopmental scores (P < 0.001). CONCLUSION: Hypothermia therapy significantly reduces serum levels of miR-21 and S-100B protein in neonatal HIE patients and may be associated with better prognosis. miR-21 and S-100B serve as prognostic biomarkers, aiding in predicting and improving the treatment outcomes and long-term prognosis of neonatal HIE.

xenoGI 3: using the DTLOR model to reconstruct the evolution of gene families in clades of microbes.

To understand genome evolution in a group of microbes, we need to know the timing of events such as duplications, deletions and horizontal transfers. A common approach is to perform a gene-tree / species-tree reconciliation. While a number of software packages perform this type of analysis, none are geared toward a complete reconstruction for all families in an entire clade. Here we describe an update to the xenoGI software package which allows users to perform such an analysis using the newly developed DTLOR (duplication-transfer-loss-origin-rearrangement) reconciliation model starting from genome sequences as input.

Chronic inflammation as a potential mediator between phthalate exposure and depressive symptoms.

BACKGROUND: A few studies have reported phthalate exposure as a risk factor for depressive symptoms, but the results have been inconsistent. Whether chronic inflammation mediates the relationship between phthalates (PAEs) and depressive symptoms remains unclear. In this study, we establish mediating models of inflammatory factors and explore the mediating role of chronic inflammation in the association between PAEs exposure and depressive symptoms. METHODS: The sample included 989 participants from the Study on Health and Environment of the Elderly in Lu'an City, Anhui Province. Geriatric depression scale (GDS-30) was used to screen depressive symptoms of the elderly. The levels of seven kinds of PAEs in urine samples and four inflammatory factors in serum of the elderly were measured. To establish the mediating effect of inflammatory factors to explore the potential effect of PAEs exposure on the increased odds of depressive symptoms. RESULTS: Adjusted for multiple variables, the highest tertiles of Mono (2-ethylhexyl) phthalate (MEHP) (95%CI = 1.051-2.112), Mono benzyl phthalate (MBzP) (95%CI = 1.016-2.082) and Mono butyl phthalate (MBP) (95%CI = 1.102-2.262) were positively correlated with depressive symptoms. The mediating effect of IL-6 and generalized inflammation factor between MEHP exposure and depressive symptoms were 15.96% (95%CI=0.0288-0.1971) and 14.25% (95%CI = 0.0167-0.1899). CONCLUSIONS: High levels of MEHP, MBzP and MBP increased the odds of depressive symptoms in the elderly, and chronic inflammation had a partial mediating effect on the increased odds of depressive symptoms due to MEHP exposure.

Microbes team with nanoscale zero-valent iron: A robust route for degradation of recalcitrant pollutants.

Integrating nanoscale zero-valent iron (nZVI) with biological treatment processes holds the promise of inheriting significant advantages from both environmental nano- and bio-technologies. nZVI and microbes can perform in coalition in direct contact and act simultaneously, or be maintained in separate reactors and operated sequentially. Both modes can generate enhanced performance for wastewater treatment and environmental remediation. nZVI scavenges and eliminates toxic metals, and enhances biodegradability of some recalcitrant contaminants while bioprocesses serve to mineralize organic compounds and further remove impurities from wastewater. This has been demonstrated in a number of recent works that nZVI can substantially augment the performance of conventional biological treatment for wastewaters from textile and nonferrous metal industries. Our recent laboratory and field tests show that COD of the industrial effluents can be reduced to a record-low of 50 ppm. Recent literature on the theory and applications of the nZVI-bio system is highlighted in this mini review.

Maximum parsimony reconciliation in the DTLOR model.

BACKGROUND: Analyses of microbial evolution often use reconciliation methods. However, the standard duplication-transfer-loss (DTL) model does not account for the fact that species trees are often not fully sampled and thus, from the perspective of reconciliation, a gene family may enter the species tree from the outside. Moreover, within the genome, genes are often rearranged, causing them to move to new syntenic regions. RESULTS: We extend the DTL model to account for two events that commonly arise in the evolution of microbes: origin of a gene from outside the sampled species tree and rearrangement of gene syntenic regions. We describe an efficient algorithm for maximum parsimony reconciliation in this new DTLOR model and then show how it can be extended to account for non-binary gene trees to handle uncertainty in gene tree topologies. Finally, we describe preliminary experimental results from the integration of our algorithm into the existing xenoGI tool for reconstructing the histories of genomic islands in closely related bacteria. CONCLUSIONS: Reconciliation in the DTLOR model can offer new insights into the evolution of microbes that is not currently possible under the DTL model.

Homocysteine induced a calcium-mediated disruption of mitochondrial function and dynamics in endothelial cells.

Homocysteine (Hcy) is a sulfur-containing amino acid that originated in methionine metabolism and the elevated level of Hcy in plasma is considered to be an independent risk factor for cardiovascular diseases (CVD). Endothelial dysfunction plays a major role in the development of CVD, while the potential mechanism of Hcy-induced endothelial dysfunction is still unclear. Here, in Hcy-treated endothelial cells, we observed the destruction of mitochondrial morphology and the decline of mitochondrial membrane potential. Meanwhile, the level of ATP was reduced and the reactive oxygen species was increased. The expressions of dynamin-related protein 1 (Drp1) and phosphate-Drp1 (Ser616) were upregulated, whereas the expression of mitofusin 2 was inhibited by Hcy treatment. These findings suggested that Hcy not only triggered mitochondrial dysfunction but also incurred an imbalance of mitochondrial dynamics in endothelial cells. The expression of mitochondrial calcium uniporter (MCU) was activated by Hcy, contributing to calcium transferring into mitochondria. Interestingly, the formation of mitochondria-associated membranes (MAMs) was increased in endothelial cells after Hcy administration. The inositol 1,4,5-triphosphate receptor (IP3R)-glucose-regulated protein 75 (Grp75)-voltage-dependent anion channel (VDAC) complex, which was enriched in MAMs, was also increased. The accumulation of mitochondrial calcium could be blocked by inhibiting with the IP3R inhibitor Xestospongin C (XeC) in Hcy-treated cells. Then, we confirmed that the mitochondrial dysfunction and the increased mitochondrial fission induced by Hcy could be attenuated after Hcy and XeC co-treatment. In conclusion, Hcy-induced mitochondrial dysfunction and dynamics disorder in endothelial cells were mainly related to the increase of calcium as a result of the upregulated expressions of the MCU and the IP3R-Grp75-VDAC complex in MAMs.

Rictor/mTORC2 involves mitochondrial function in ES cells derived cardiomyocytes via mitochondrial Connexin 43.

Rictor is a key component of the mammalian target of rapamycin complex 2 (mTORC2) and is required for Akt phosphorylation (Ser473). Our previous study shows that knockdown of Rictor prevents cardiomyocyte differentiation from mouse embryonic stem (ES) cells and induces abnormal electrophysiology of ES cell-derived cardiomyocytes (ESC-CMs). Besides, knockdown of Rictor causes down-expression of connexin 43 (Cx43), the predominant gap junction protein, that is located in both the sarcolemma and mitochondria in cardiomyocytes. Mitochondrial Cx43 (mtCx43) plays a crucial role in mitochondrial function. In this study, we used the model of cardiomyocyte differentiation from mouse ES cells to elucidate the mechanisms for the mitochondrial damage in ESC-CMs after knockdown of Rictor. We showed swollen and ruptured mitochondria were observed after knockdown of Rictor under transmission electron microscope. ATP production and mitochondrial transmembrane potential were significantly decreased in Rictor-knockdown cells. Furthermore, knockdown of Rictor inhibited the activities of mitochondrial respiratory chain complex. The above-mentioned changes were linked to inhibiting the translocation of Cx43 into mitochondria by knockdown of Rictor. We revealed that knockdown of Rictor inactivated the mTOR/Akt signalling pathway and subsequently decreased HDAC6 expression, resulted in Hsp90 hyper-acetylation caused by HDAC6 inhibition, thus, inhibited the formation of Hsp90-Cx43-TOM20 complex. In conclusion, the mitochondrial Cx43 participates in shRNA-Rictor-induced mitochondrial function damage in the ESC-CMs.

Inferring Pareto-optimal reconciliations across multiple event costs under the duplication-loss-coalescence model.

BACKGROUND: Reconciliation methods are widely used to explain incongruence between a gene tree and species tree. However, the common approach of inferring maximum parsimony reconciliations (MPRs) relies on user-defined costs for each type of event, which can be difficult to estimate. Prior work has explored the relationship between event costs and maximum parsimony reconciliations in the duplication-loss and duplication-transfer-loss models, but no studies have addressed this relationship in the more complicated duplication-loss-coalescence model. RESULTS: We provide a fixed-parameter tractable algorithm for computing Pareto-optimal reconciliations and recording all events that arise in those reconciliations, along with their frequencies. We apply this method to a case study of 16 fungi to systematically characterize the complexity of MPR space across event costs and identify events supported across this space. CONCLUSION: This work provides a new framework for studying the relationship between event costs and reconciliations that incorporates both macro-evolutionary events and population effects and is thus broadly applicable across eukaryotic species.

8-bromo-7-methoxychrysin suppress stemness of SMMC-7721 cells induced by co-culture of liver cancer stem-like cells with hepatic stellate cells.

BACKGROUND: Our previous works have demonstrated that 8-bromo-7-methoxychrysin suppressed stemness of human hepatocellular carcinoma (HCC) cell line SMMC-7721 induced by condition medium from hepatic stellate cell line LX-2 that was activated by liver cancer stem-like cells (LCSCs). However, whether and whereby BrMC inhibits the stemness induced by co-culture of LCSCs and LX-2 cells remains to be investigated. METHODS: The second-generation spheres by sphere culture were identified and used as SMMC-7721-and MHCC97H-derived LCSLCs. SMMC-7721-and MHCC97-derived LCSCs/LX-2 cells transwell co-culture system was treated with BrMC and its lead compound chrysin. The concentrations of IL-6, IL-8, HGF and PDGF in condition medium from co-culture were measured by enzyme-linked immunosorbent assay (ELISA). The stemness of SMMC-7721 cells was evaluated by sphere formation assay and western blot analysis for expression levels of cancer stem cell markers (CD133 and CD44).The expression levels of cancer-associated fibroblast markers (FAP-α and α-SMA) were employed to evaluate pathologic activation of LX-2 cells. Addition of IL-6 and/or HGF or deletion of IL-6 and/or HGF was conducted to investigate the mechanisms for BrMC and chrysin treatment in SMMC-7721-derived LCSLCs co-cultured with LX-2cells. RESULTS: The co-culture of LCSLCs with LX-2 cells increased sphere formation capability as well as expression of CD133 and CD44 in SMMC-7721 cells, meanwhile, upregulated expression of FAP-α in LX-2 cells. ELISA indicated that the concentrations of IL-6 and HGF were significantly elevated in Co-CM than that of condition media from co-cultured SMMC-7721 cells/LX-2 cells. Treatment of BrMC and chrysin with co-cultures of SMMC-7721- and MHCC97H-derived LCSLCs and LX-2 cells effectively inhibited the above responses. Moreover, addition of IL-6 and/or HGF induced stemness of SMMC-7721 cells and activation of LX-2 cells, conversely, deletion of IL-6 and/or HGF suppressed those. Furthermore, the inhibitory effects of BrMC and chrysin on stemness of SMMC-7721 cells and activation of LX-2 cells were attenuated by addition of IL-6 or HGF, and enhanced by deletion of IL-6 or HGF. CONCLUSIONS: Our results suggest IL-6 and HGF may be the key communication molecules for the interaction between LCSLCs and HSCs, and BrMC and chrysin could block these effects and be the novel therapeutic candidates for HCC management.

Geochemical simulation of the stabilization process of vanadium-contaminated soil remediated with calcium oxide and ferrous sulfate.

Vanadium (V)-contaminated soil poses health risks to plants, animals, and humans via both direct exposure and through the food chain. Stabilization treatment of metal-contaminated soil can chemically convert metal contaminants into less soluble, mobile, and toxic forms. However, the stabilization mechanisms of V-contaminated soil have not been thoroughly investigated. Therefore, we performed geochemical modeling of V-contaminated soil stabilized with the common binders calcium oxide (CaO) and ferrous sulfate (FeSO4), as well as their mixture, using Visual MINTEQ software. The results were validated and exhibited good agreement with experimental results. For CaO, the formation of Ca2V2O7(s) and Ca3(VO4)2·4H2O(s) under mild and strong alkaline conditions (pH = 8.0-11.5 and 11.5-12.5), respectively, were predicted as the main immobilization routes. For FeSO4, there appeared to be three reaction routes, corresponding to approaches A, B, and C, during the stabilization process. In the simulation, approach C (adsorption of V(V) onto ferrihydrite) was undervalued, whereas approaches A (formation of Fe(VO3)2(s)) and B (reduction of V(V) into V(IV) to form V2O4(s) or adsorb onto soil organic matter) were overvalued. Among the three approaches, approach C had a dominant role and exhibited good agreement with the experimental results. Additionally, soil pH and the saturation index of precipitation had major roles in the stabilization process. The optimal pH ranges for the stabilization of V-contaminated soil using CaO and FeSO4 were pH = 9.5-12.5 and pH = 4.0-5.0, respectively.

Vanadium and chromium-contaminated soil remediation using VFAs derived from food waste as soil washing agents: A case study.

Food waste (FW) is environmentally unfriendly and decays easily under ambient conditions. Vanadium (V) and chromium (Cr) contamination in soils has become an increasing concern due to risks to human health and environmental conservation. Volatile fatty acids (VFAs) derived from FW was applied as soil washing agent to treat V and Cr-contaminated soil collected from a former V smelter site in this work. The Community Bureau of Reference (BCR) three-step sequential extraction procedure was used to identify geochemical fractions of V and Cr influencing their mobility and biological toxicity. Optimal parameters of a single washing procedure were determined to be a 4 h contact time, liquid-solid ratio of 10:1, VFAs concentration of 30 g/L, and reaction temperature of 25 °C, considering for typical soil remediation projects and complete anaerobic fermentation of FW. Under the optimal conditions, butyric acid fermentation VFAs attained removal rates of 57.09 and 23.55% for extractable fractions of V and Cr, respectively. Simultaneously, a multi-washing process under a constant liquid-solid ratio using fresh and recycled VFAs was conducted, which led to an improvement on the total removal efficiency of toxic metals. The washing procedure could reach the pollution thresholds for several plants, such as of S. viridis, K. scoparia, M. sativa, and E. indica. This strategy enhances the utilization of VFAs derived from food waste, has a positive effect on V and Cr-contaminated soil remediation, wastewater control of soil washing and FW disposal.

Biological denitrification from mature landfill leachate using a food-waste-derived carbon source.

The mature landfill leachate containing high ammonia concentration (>1000 mg/L) is a serious threat to environment; however, the low COD to TN ratio (C/N, <3) strongly inhibits the denitrification process and poses a severe obstacle for efficient treatment. Herein, two kinds of acidogenic liquids, fermented from oil-removed food waste and oil-added food waste, were first applied as external carbon sources for the biological nitrogen removal from mature landfill leachate in an aerobic/anoxic membrane bioreactor. "Acidogenic liquid b" served quite better than commercial sodium acetate, considering the higher denitrification efficiency and the slightly rapider denitrification rate. The effect of C/N and temperature were investigated under hydraulic retention time (HRT) of 7 d, which showed that C/N ≥ 7 (25 °C) was enough to meet the general discharge standards of NH4+-N, TN and COD in China. Even for some special areas of China, the more stringent discharge standards (NH4+-N ≤ 8 mg/L, TN ≤ 20 mg/L) could also be achieved under longer HRT of 14 d and C/N ≥ 6. Notably, the COD concentration in effluent could also be well reduced to 50-55 mg/L, without further physical-chemical treatment. This proposed strategy, involving the high-value utilization of food waste, is thus promising for efficient nitrogen removal from mature landfill leachate.

Enhancement of volatile fatty acid production and biogas yield from food waste following sonication pretreatment.

The positive effect of sonication on volatile fatty acid (VFA) and hydrogen production was investigated by batch experiments. Several sonication densities (2, 1.6, and 1.2 W/mL) and times (5, 10, and 15 min) were tested. The optimal sonication condition was ultrasonic density 2 W/mL and ultrasonic time 15 min (2-U15). The FW particle size larger than 50 µm (d > 50 µm) were more susceptible to the sonication treatment than the smaller particle size (d ≤ 50 µm). The SCOD increased and VS reduction accelerated under sonication treatment. The maximum VFA production and the highest proportion of hydrogen in the biogas increased 65.3% and 59.1%, respectively, under the optimal sonication conditions compared to the unsonicated batch. Moreover, a reduction of over 50% in the time required to reach its maximum production was also observed. Butyric acid fermentation type was obtained whether following sonication treatment or not. The composition of key microbial community differed under the various sonication conditions. The genera Clostridium and Parabacteroides are predominantly responsible for VFA generation and both were found to be abundant under the optimal condition.

The interactions of metal concentrations and soil properties on toxic metal accumulation of native plants in vanadium mining area.

High demand of Vanadium (V) in high-strength steel and battery manufacturing industry led to extensive V mining activity in China, and caused multi-metal pollution of soil around V mining area. To understand the phytoremediation potentials of native plants grown in V mining area, and the effect of soil properties and soil metal concentrations on toxic metal accumulations of native plants. Setaria viridis, Kochia scoparia and Chenopodium album were sampled from different sites in V mining area, soil properties, soil metal concentrations and metal accumulation amount of investigated plants were measured, bioaccumulation (BAF) and translocation (TF) efficiencies were calculated. Soil pH, cation exchange capacity (CEC) and available phosphorous (P) can significantly affect V and copper (Cu) uptake in the shoots of Setaria viridis while soil metal contents were lower than the permissible limits. Soil pH can significantly affect V accumulations in the roots and shoots of Kochia scoparia grown in slightly V polluted soils. Setaria viridis exhibited TF > 1 for moderately V and slightly chromium (Cr) polluted soils, and BAF>1 for slightly Cu contaminated soils respectively. Kochia scoparia and Chenopodium album showed TF > 1 and BAF>1 for slightly V polluted soils, respectively. Setaria viridis was practical for in situ phytoextractions of moderately V and slightly Cr polluted soils, and phytostabilization of slightly Cu contaminated soils. Kochia scoparia and Chenopodium album could be used as phytoextractor and phytostablizer in slightly V polluted soils in V mining area. Metal uptake of native plants grown in slightly multi-metal contaminated sites in V mining area can be manipulated by altering soil properties.

Green Synthesis of Nanosilica from Coal Fly Ash and Its Stabilizing Effect on CaO Sorbents for CO2 Capture.

High-temperature sorption of CO2 via calcium looping has wide applications in postcombustion carbon capture, sorption-enhanced hydrogen production, and inherent energy storage. However, fast deactivations of CaO sorbents and low CO2 uptake in the fast carbonation stage are major drawbacks of this technology. For the first time, we developed a green approach through the reuse of nanosilica derived from coal fly ash (CFA) to enhance both the cyclic CO2 uptakes and the sorption kinetics of CaO sorbents. The as-synthesized nanosilica-supported CaO sorbent showed superior cyclic stability even under realistic carbonation/calcination conditions, and maintained a final CO2 uptake of 0.20 g(CO2) g(sorbent)-1 within short carbonation time, markedly increased by 155% over conventional CaO sorbent. Significantly, it also exhibited very fast sorption rate and could achieve almost 90% of the total CO2 uptake within ∼20 s after the second cycle, which is critical for practical applications. These positive effects were attributed to the formation of larnite (Ca2SiO4) and the physical nanostructure of silica, which could yield and keep abundant reactive small pores directly exposed to CO2 throughout multiple cycles. The proposed strategy, integrating the on-site recycling of CFA, appears to be promising for CO2 abatement from coal-fired power plants.

Controlling odors from sewage sludge using ultrasound coupled with Fenton oxidation.

We examined the effects of ultrasound (U), Fenton oxidation (F), and ultrasound coupled with Fenton oxidation (U + F) pre-treatments (prior to anaerobic digestion) on the elimination of odorous compounds. The results demonstrated that U promoted odor release, while the coupled treatment and F alone decreased odor release. After 20-min treatments, the concentration of dissolved sulfide (S(2-)) under the coupled U + F treatment declined from 17.4 mg/L to 8.1 mg/L, decreasing by more than 50% and 34%, respectively, for U alone and F alone. In addition, the dissolved sulfate (SO4(2-)) concentration under couple U + F treatment significantly increased in sewage sludge from 200 mg/L to 390.6 mg/L, up 95.3% compared to U alone and 5% compared to F alone. This illustrates the oxidation process from S(2-) to SO4(2-). Throughout experimentation, SO4(2-) was odorless and stable, highlighting the mechanism of odor control. Thus, combining U and F into a single coupled treatment proved to be a better alternative pretreatment for controlling sludge odor compared to the U and F alone and can effectively decrease potential odor release.

Controllable Construction of a Mo2C/MoO2 Interface with an Ideal Mo2C/MoO2 Ratio for Efficient Electrocatalytic Nitrogen Reduction to Ammonia.

Electrocatalytic nitrogen reduction reaction (NRR) is considered to be a viable contender for the production of NH3. However, due to the sluggish adsorption and activation of the electrocatalyst toward inert N2 molecules, there is an urgent need for developing effective catalysts to facilitate the reaction. Inspired by natural nitrogenase, in which Mo atoms are the active centers, Mo-based electrocatalysts have received considerable attention, but further exploration is still necessary. Interface-engineered electrocatalysts can effectively optimize the absorption and activation of the catalytic active center for N2 and thus improve the electrocatalytic activity of NRR. However, the lack of studies for controllably constructing an optimal ratio of two phases at the interface hinders the development of NRR electrocatalysts. Herein, a series of Mo2C/MoO2 interface-engineered electrocatalysts with various Mo2C/MoO2 ratios were constructed by controlling the Y dosages. The controlled experimental results verified that the catalytic activity of NRR, the dosage of Y, and the ratio of Mo2C/MoO2 were strongly correlated. Density functional theory calculations show that the C-Mo-O coordination at the Mo2C/MoO2 interface can optimize the reaction path and reduce the energy barrier of the reaction intermediates, thereby enhancing the reaction kinetics of NRR.