SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
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IF 5.107
Hao Ling,Sen Liu,Hongxia Gao,Haiyan Zhang,Zhiwu Liang
In order to establish an integrative mass transfer coefficient (K G a V ) model for CO 2 absorption into blended monoethanolamine (MEA)/1-dimethylamino-2-propanol (1DMA2P) solution in packed column, the models of CO 2 Henry’s law constants (He CO₂-MEA/1DMA2P ) and the equilibrium CO 2 solubility (α eq ) were constructed. The experimental produced data can be reasonably analyzed. In this work, the Arrhenius equation was employed to fit the values of He CO₂-MEA/1DMA2P at different temperature with AARD of 4.06%; the Kent-Eisenberg prediction model and empirical polynomial prediction model were used to predict the data of α eq under different CO 2 partial pressures and temperatures with AARDs of 2.64% and 0.83%, respectively; the empirical K G a V model proposed by Li, the empirical K G a V model proposed by Aroonwilas and new K G a V model were used to correlate the average values of K G a V with AARDs of 14.36%, 12.44% and 9.03%, respectively; the model for outlet CO 2 concentration (y CO₂,out ) in packed column was developed with AARD of 15.97%. Moreover, the heat of CO 2 absorption in 6 kmol/m 3 MEA/1DMA2P solution was estimated by Gibbs-Helmholtz equation which gave a value of −39.8 kJ/mol. The results show that the blended MEA/1DMA2P solution has advantages that make it a potential absorbent for CO 2 capture.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Zhe Li,Yunshuo Wu,Haiqiang Wang,Zhongbiao Wu,Xuanhao Wu
Nitrous oxide (N2O) is a potent greenhouse gas with a high global warming potential, emphasizing the critical need to develop efficient elimination methods. Electrocatalytic N2O reduction reaction (N2ORR) stands out as a promising approach, offering room temperature conversion of N2O to N2 without the production of NOx byproducts. In this study, we present the synthesis of a copper-based single-atom catalyst featuring atomic Cu on nitrogen-doped carbon black (Cu1–NCB). Attributed to the highly dispersed single-atom Cu sites and the effective suppression of the hydrogen evolution reaction, Cu1–NCB demonstrated an optimal N2 faradaic efficiency (82.1%) and yield rate (3.53 mmol h–1 mgmetal–1) at −0.2 and −0.5 V vs RHE, respectively, outperforming previously reported N2ORR electrocatalysts. Further, a gas diffusion electrode cell was employed to improve mass transfer and achieved a 28.6% conversion rate of 30% N2O with only a 14 s residence time, demonstrating the potential for practical application. Density functional theory calculations identified Cu–N4 as the crucial active site for N2ORR, highlighting the significance of the unsaturated coordination and metal–support electronic structure. O-terminal adsorption of N2O was favored, and the dissociative adsorption (*ON2 → *O + N2) was the rate-determining step. These findings reveal the broad prospects of N2O decomposition via electrocatalysis.
研究领域:
环境科学
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催化
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电化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Nitrogen
·
2025
·Vol. 6
·期 3
·57
·
IF 2.3
Shutan Ma,Jintao Zhang,Ting Wu,Yuqing Miao,Hua Fang,Haitao Wang,Huayuan Niu,Lan Ma
The substrate-induced respiration-inhibition (SIRIN) method has been used to estimate fungi-derived N2O emissions, but its contribution to soil N2O emissions remains unclear. There is a need to quantify the fungal fraction of N2O production more precisely. Here, using isotopocule analysis, we assessed the relative contribution of fungi to soil N2O production potential under denitrifying conditions, where key limiting factors of denitrification (soil moisture, soil NO3−, and electron donor) were removed. The result showed that the ratio of fungi-derived N2O emissions (RF) was 0.83~4.28% in paddy soils, 13.80~23.21% in vineyard soils, and 15.34~65.94% in vegetable field soils, respectively. This indicated that the bacteria were the dominator of soil N2O production potential in most cases, but fungal pathways could be significant in vegetable field soils. The experiment with bactericide addition showed that inhibitors could affect non-target microorganisms in the SIRIN method. Our further analyses suggest that it is worth to explore the effect of soil organic carbon and microbial synergies on fungi-derived N2O emissions.
研究领域:
土壤科学
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微生物生态学
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环境科学
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农业科学
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产品关联
DOI
高影响因子
CHEMOSPHERE
·
2019
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IF 5.108
Peng Yan,Kai Li,Jin-Song Guo,Si-Xi Zhu,Zhi-Kang Wang,Fang Fang
A dynamic analysis approach for determining nitrite production and consumption rates was established to systematically investigate the characteristics of nitrogen transformation and N 2 O emission of the completely autotrophic nitrogen removal over nitrite (CANON) process coupled with denitrification using a sequencing batch biofilm reactor (SBBR). The results indicate that anaerobic ammonium-oxidizing bacteria was not inhibited significantly by low C/N ratios. There were no obvious differences in the nitrite production rate, nitrite consumption rate or nitrogen removal among reactors operated with C/N ratios of 0, 0.67 and 1.00, which suggested that the certain carbon source did not significantly affect the nitrite conversion and nitrogen removal in the process. More than 60% of total N 2 O emission is generated during the initial phase of each period in the SBBR. More than 94.5% of N 2 O was generated by NO 2 − -N consumption via denitrification in the process. Interestingly, total N 2 O production drops by 16.7%, when the C/N ratio increases from 0 to 1. This phenomenon may be caused by the inhibition of N 2 O production via AOB denitrification. Therefore, an appropriate carbon source (C/N = 1.00) has the beneficial effect of reducing N 2 O emission by CANON coupled with denitrification. The results of this study provide an important empirical foundation for the mitigation of N 2 O emission in the CANON process coupled with denitrification.
研究领域:
环境工程
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微生物学
·
污水处理
✓ 已验证
DOI
PubMed
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2021
·
IF 6.291
Rui Tao,Hanjie Zhang,Xiuping Gu,Baowei Hu,Jun Li,Guixin Chu
Phthalic acid esters (PAEs) pollution has become an increasing issue worldwide, but little is known about its effects on ammonia-oxidizers and nitrous oxide (N 2 O) in the soil environment. Here, a 50-day soil microcosm experiment was conducted using low and high doses bis (2-Ethylhexyl) phthalate (DEHP) to estimate the effect of DEHP exposure on soil N 2 O emissions and the nitrifying community in calcareous soil. The results showed that DEHP exposure at 10 and 100 mg kg -1 doses significantly reduced N 2 O by 67.5% and 73.6%, respectively, relative to the DEHP absent treatment. The microbial biomass carbon and nitrogen (MBC and MBN) were consistently and significantly decreased with DEHP exposure at 5, 22, and 50 days after incubation, especially with high-dose. The bipartite association networks showed that DEHP exposure changed the compositions of both ammonia-oxidizing archaea (AOA) and ammonia-oxidizing bacteria (AOB) communities. Moreover, the AOA and AOB amoA gene abundances were significantly decreased by DEHP addition to the soil ( P < 0.05). Random forest modeling showed that the AOB Shannon index and pH were the most important biotic and abiotic factors affecting N 2 O emissions in the soil with DEHP exposure, respectively. Partial least squares path modeling (PLS-PM) demonstrated that the reduction of N 2 O emissions due to DEHP exposure was mainly ascribed to the changes of the AOB community. The results from this study highlight the toxicity of DEHP on the ammonia oxidizers, and its mitigating effect on N 2 O emissions in the soil where ammonia-oxidation is largely driven by AOB.
研究领域:
环境科学
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土壤微生物学
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生态毒理学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF SOILS AND SEDIMENTS
·
2026
·Vol. 26
·期 10
·351
·
IF 3.3
Gao Fuyun,Liu Xinhui,Zeng Jieyi,Li Yaying,Yao Huaiying
Purpose The chemical form of zinc is a critical determinant of its behaviour in soil, yet its specific role in regulating microbial nitrogen cycling and nitrous oxide (N 2 O) emissions remains inadequately understood. This study investigated the dose-dependent effects of zinc oxide nanoparticles (ZnO NPs) and zinc sulfate (ZnSO 4 ) on soil N 2 O emissions and microbial nitrogen cycling in the acidic agricultural soil. Materials and methods Gas chromatography and high-throughput sequencing were used to explore the effects of two types of Zn fertilizers (ZnO NPs and ZnSO 4 ) and four additional doses (10, 50, 100, and 500 mg kg − 1 ) on N 2 O emissions in soil from a rice–wheat rotational system. Results and discussion Through controlled microcosm experiments, we demonstrated that the use of ZnO NPs at concentrations ≥ 50 mg kg − 1 significantly reduced cumulative N 2 O emissions (4.33–28.53%). High concentrations (500 mg kg − 1 ) of ZnO NPs inhibited soil ammonia monooxygenase and nitrite reductase activities and reduced the abundance of archaeal ammonia oxidizers (AOA) amoA and nirS genes, and the relative abundance of Nitrososphaerales, which was the key factor leading to a decrease in N 2 O emissions. ZnSO 4 exhibited stronger inhibition (14.1% reduction at 500 mg kg − 1 ) because of its higher zinc ion (Zn 2+ ) bioavailability, highlighting nanoparticle dissolution kinetics as a critical regulatory factor. Soil bacterial microbial community structure under low concentration (10 mg kg − 1 ) of ZnO NPs differed from other treatments. The soil bacterial community structure differed from that in the other treatments under a low concentration (10 mg kg − 1 ) of ZnO NPs. Compared with their bacterial counterparts (AOB), AOA were more sensitive to ZnO NPs, which aligns with the results of pH-dependent niche partitioning in acidic soils. Conclusion Overall, optimal ZnO NPs and ZnSO 4 application mitigated agricultural N 2 O emissions. These findings underscore the potential of strategically applied ZnO NPs to mitigate N 2 O emissions and promote the sustainable use of nanofertilizers.
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DOI
高影响因子
ACS ES&T Engineering
·
2024
·
IF 7.4
Zhuoyi Zhang,Yunshuo Wu,Yuxin Sun,Haiqiang Wang,Zhongbiao Wu,Xuanhao Wu
Nitrous oxide (N2O) is a potent greenhouse gas with a high global warming potential. The N2O direct decomposition (deN2O) is currently the most widely used technique due to its operational simplicity and lack of secondary pollution. The presence of impurity gases in industrial exhaust increases the challenge of eliminating N2O, urging the development of highly active and stable catalysts for its degradation. In this study, a series of praseodymium (Pr)-doped nickel oxide (NiO) catalysts were synthesized for N2O degradation. These catalysts showed higher N2O decomposition activity (T100 = 400–440 °C) than pure NiO (T100 = 480 °C) and also demonstrated high resistance to impurity gases in simulated industrial nitric acid tail gas. In the catalyst with a Pr to Ni ratio of 0.002, the highly dispersed Pr on the NiO surface regulated its particle size and increased specific surface area and pore volume. DFT calculations revealed that Pr significantly enhanced the electron-donating ability of Ni2+, facilitating the dissociative adsorption of N2O on the catalyst surface, where O existed in the form of Ni3+-O*. Additionally, Pr reduced the desorption energy of O2, the rate-determining step. During the reaction, Pr3+ transferred electrons to Ni3+ via f-d electron hopping, stabilizing the active Ni2+ sites and enabling an efficient catalytic reaction. These findings demonstrate the practical potential of this catalyst and provide new insights into the degradation of N2O in industrial exhaust gases, offering a promising avenue for application.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2026
·
IF 6.3
Minghui Chen,Yanxia Gao,Haiqiang Wang,Zhongbiao Wu,Xuanhao Wu
Abstract Photothermal catalysis offers a light-driven route for N2O abatement by coupling broadband light harvesting with catalytic surface reactions. Here, spinel Co3O4 catalysts were prepared by calcining at 400, 500, and 600 °C (denoted as Co3O4-400, Co3O4-500, and Co3O4-600, respectively). This temperature-controlled synthesis preserved the spinel framework while modulating the local bonding environment surrounding the Co centers. Among the three catalysts, Co3O4-500 exhibited a relatively less-coordinated octahedral Co–O–Co environment, accompanied by modest surface Co2+ enrichment. Light-assisted N2O temperature-programmed desorption showed that Co3O4-500 retained a larger population of thermally stable N2O-related species, while in situ infrared spectroscopy revealed more rapid attenuation of the bands assigned to N–N- and N–O-related vibrations under illumination. Temperature-matched controls further showed that its enhanced activity could not be explained by macroscopic catalyst-bed heating alone. Accordingly, Co3O4-500 achieved 93.5% single-pass N2O conversion and a decomposition rate of 40.82 mmol g–1 h–1 at 1.81 W cm–2 under broadband irradiation. These results associate the photothermal activity of Co3O4 with its local Co–O coordination environment and identify coordination regulation through controlled thermal treatment as a strategy for designing non-noble-metal catalysts for N2O abatement.
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Shuang Cao,Zhuoyi Zhang,Yunshuo Wu,Yuxin Sun,Zhe Li,Yanxia Gao,Haiqiang Wang,Xuanhao Wu,Zhongbiao Wu
Nitrous oxide (N 2 O) is a potent greenhouse gas with high global warming potential. It is urgent to develop active and stabile catalysts for N 2 O direct catalytic decomposition (deN 2 O) in industrial exhaust gas. In this study, a series of Eu-doped NiO catalysts were synthesized by co-precipitation method. The catalyst with an Eu to Ni molar ratio of 0.04 showed the highest deN 2 O ability, reaching 100 % conversion at 400 °C without generating NO x by-products. The catalyst also displayed resilience against O 2 and NO impurity gases, maintaining structural stability and achieving complete transformation of N 2 O at 440 °C. Eu was uniformly dispersed in NiO in the form of Eu 2 O 3 , which not only regulated the particle size and specific surface area of NiO, but also changed the surface chemistry of NiO by inducing more Ni 2+ active sites and more mobile O β species. Eu-doping altered the decomposition mechanism of N 2 O from L-H to E-R mechanism, reducing the energy barrier of O 2 desorption, which was the rate-determining step. During the reaction, Eu 0.04 Ni showed an activation behavior after cyclic use and long-term reaction and reduced T 100 to 320 °C after 14-hr experiment. These findings demonstrate the potential of the catalyst for practical application and provide new routes for the direct decomposition of N 2 O in industrial exhaust gas.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2018
·
IF 3.525
Lei Chen,Ding Weng,Jiadao Wang,Duan Weng,Li Cao
The CeO 2 -TiO 2 (CeTi) and CeO 2 /WO 3 -TiO 2 (CeWTi) catalysts were prepared by a sol-gel precipitation method and their NH 3 -NO/NO 2 selective catalytic reduction (SCR) performance was studied. N 2 O formation and effect of oxygen concentration on SCR performance over CeWTi catalyst were also investigated while varying the NO 2 /NO x ratio. Results indicate that fast SCR behavior of CeWTi catalyst has the best NH 3 -NO/NO 2 SCR performance due to the catalyst reoxidation rate by NO 2 higher than by O 2 . Compared with CeTi catalyst, CeWTi catalyst exhibits higher de-NO x performance under NH 3 -NO/NO 2 SCR conditions. As the CeTi and CeWTi catalysts exhibit similar redox property, addition of WO 3 provides more acid sites which accelerate the reaction between NH 4 NO 3 and NO to get a superior low-temperature activity. Amount of N 2 O formation shows a peak at 250 °C mainly derived from NH 4 NO 3 decomposition.
研究领域:
催化劑科學
·
環境工程
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2018
·
IF 5.807
Zhengsong Wu,Fei Xu,Chun Yang,Xiaoxuan Su,Fucheng Guo,Qinyuan Xu,Guilong Peng,Qiang He,Yi Chen
Biochar is widely used in water treatment because of its porous structure, however, the effects of biochars on denitrification remain unclear. Here, we combined molecular biological and electrochemical techniques to investigate effects of biochars (formed at 300 °C, 500 °C and 800 °C) on denitrification. Results showed that biochar at 300 °C increased total nitrogen removal by 415% and decreased N 2 O accumulation by 78%. Mechanistic research demonstrated that it achieved the highest electron transfer efficiency and denitrifying enzyme activities. Further study evidenced that biochar at 300 °C increased the abundance of denitrifiers such as Pseudomonas . Correlation analysis indicated that nitrate reductase and nitrite reductase activities were the key factors influenced by biochar during denitrification. Overall, this study suggested that biochar at 300 °C could act as the bio-engineer of electron shuttle and the stimulator of denitrification, achieving high rate nitrogen removal and significant reduction of N 2 O accumulation from high-strength wastewater.
研究领域:
环境科学
·
微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2024
·
IF 5.2
Ziheng Zhen,Antai Li,Youwei Yang,Ying Hu,Jing Lv,Shouying Huang,Yue Wang,Xinbin Ma
Cu/CeO 2 catalysts have been wildly used for the hydrogenation of carbon-oxygen bonds reactions due to their excellent catalytic performance. It is widely accepted that the Cu 0 -Cu σ+ interface could be the primary active sites during the reaction, but how to form and maintain highly dispersed such species remains challenging under the reaction conditions of high temperature and H 2 partial pressure. In this work, we proposed an effective strategy to construct stable Cu 0 -Cu σ+ interface sites over the Cu/CeO 2 catalysts by in situ N 2 O-involved oxidation treatment . It was evidenced that the sequential oxidation-reduction by N 2 O and H 2 broke the grain boundaries of Cu nanoparticles and therefore facilitated the formation of the active Cu 0 -Cu σ+ sites, leading to an enhanced activity. However, a rapid deactivation was observed after this temporary enhancement due to the aggregation of copper species. We further introduced some additional cerium species during catalyst preparation. The 16Cu/CeO 2 -1Ce catalyst prepared by post-impregnation of 1 wt% cerium achieved a stable performance of 90.6% MA conversion after the N 2 O-involved oxidation treatment, which was much higher than that of 26.2% over the 16Cu/CeO 2 catalyst. It was demonstrated that the strong interaction between the formed CeO 2 and reconstructed Cu species prevented the metal sintering and increased the fraction of the Cu 0 -Cu σ+ sites. This method that combined in situ N 2 O-involved oxidation treatment and cerium modification may offer potential in engineering stable active sites for high-performance catalysts in the hydrogenation of carbon-oxygen bonds.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子