Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Zhiwei Dong,Yudong Ding,Fei Chen,Xun Zhu,Hong Wang,Min Cheng,Qiang Liao
The inefficient conversion of carbon dioxide (CO 2 ) to methane often restricts the advancement of CO 2 biomethanation technologies . This study explored the degrading performance, microbial community compositions, and functional gene abundance to examine the impact of zirconium metal-organic frameworks (Zr-MOFs) on the CO 2 biomethanation process. The results showed that the maximum utilization rates of CO 2 and H 2 increased by 2.77 times and 2.36 times after the addition of Zr-MOFs, respectively, and the corresponding conversion rate of CO 2 to methane also increased by 57.53%. Additionally, Zr-MOFs enhanced the COD removal efficiency and hydrolysis of tryptophan-like proteins and humic acid-like substances, resulting in more volatile organic compounds, such as tetradecane, 2-pentanone, and hexadecanoic acid. The analysis of microbial community structure revealed that the relative abundance of Methanothrix and Metanobacterium increased by 24.40% and 36.02% after the addition of Zr-MOFs, respectively. The methane metabolism revealed that Metanobacterium was a member of the same aceticlastic methanogenic pathway as Metanothrix , which encodes acetyl-CoA synthetase to catalyze the synthesis of acetyl-CoA from acetate, and Zr-MOFs also increased the relative abundance of genes that encode the enzyme responsible for converting intermediates to methane. Finally, Zr-MOFs improved the biogenesis and utilization of acetate and hydrogen (H 2 ) by enhancing the activity of enzymes, thereby providing more nutrients for methanogenesis . This study provided thorough explanations for the application and improvement of Zr-MOFs in CO 2 biomethanation technology.
研究领域:
环境生物学
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微生物学
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生物技术
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Zhanbo Guo,Chao Feng,Zongnan Shen,Xun Deng,Xinrong Feng,Min Deng,Jie Liu,Wenju Jiang,Lin Yang,Lu Yao,Zhongde Dai
Membranes have been considered as promising alternatives for natural gas sweetening. Mixed matrix membranes (MMMs) possess superior gas separation performance and the potential to combine varieties of polymers and filler materials. In the current work, MMMs have been fabricated via employing Tröger’s base (TB) polymer and zeolites with three different morphologies. Simultaneously, CO2/CH4 and H2/CH4 separation performances of the obtained MMMs were comprehensively investigated. It is found out that the presence of the MFI-type zeolites significantly improved the gas permeability, but the selectivity was somehow reduced. Among the three different nanofillers, nanosheet zeolite-based MMMs presented the highest gas permeability; with 20 wt % nanosheet zeolites, both CO2 and H2 permeabilities were increased to 348.6 and 441.5 Barrer, which were improved by 522.0 and 256.2%, respectively. In addition, SEM, XRD, FTIR, and TGA were also employed to characterize the obtained MMMs.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Dewang Zeng,Chen Wang,Tong Liu,Wentao Ou,Rui Xiao
Chemical looping methane oxidative coupling is a promising method to directly convert methane to C 2 products but is limited by the trade-off between CH 4 conversion and C 2 selectivity. Here, we develop a series of TiO 2 doped Na 2 WO 4 /Mn 2 O 3 /SiO 2 for chemical looping methane oxidative coupling and investigate the underline mechanism for the enhanced performance. The results show that 5 wt% TiO 2 doped Na 2 WO 4 /Mn 2 O 3 /SiO 2 exhibited 31.2% CH 4 conversion, which is 1.68 times as large as that of Na 2 WO 4 /Mn 2 O 3 /SiO 2 , without significantly decreasing C 2 selectivity (~70.3%). Pulse experiments show that TiO 2 improves the bulk oxygen diffusion, providing more surface oxygen to convert methane, thus leading to enhanced CH 4 conversion. O 1 s spectra manifests that the active oxygen content on the surface was not significantly increased by TiO 2 dopant , thus TiO 2 dopant has little effect on C 2 selectivity. Therefore, 5 wt% TiO 2 doped Na 2 WO 4 /Mn 2 O 3 /SiO 2 shows high chemical looping methane oxidative coupling performance. The explored mechanism in this work can be extended to design more oxygen carriers to enhance the chemical looping reactions.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Shan Gao,Tinghong Lu,Xiaohan Zhu,Fengli Yu,Bing Yuan
A catalytic system of Ru nanoparticles (NPs), Ru@SLSaq, dispersed in water was developed by employing sodium lignosulfonate (SLS) to reduce and stabilize ruthenium(III) cation heptaacetate (Ru3O(OAc)7) in an aqueous solution. This Ru@SLSaq catalytic system enabled the efficient hydrogenation of diphenylmethane (DPM) and o-hydroxydiphenylmethane (o-HDPM), yielding dicyclohexylmethane (DCHM) and perhydrofluorene (PHF), respectively. Characterization using UV–vis, FT-IR, Raman spectroscopy, HR-TEM, CO chemisorption, DLS, XRD, and XPS demonstrated that SLS effectively replaces the axial acetate ligands of Ru3O(OAc)7, reduces Ru in situ through the phenolic hydroxyls in its macromolecular structure, and maintains the stability of its core structure, thereby preventing the aggregation of generated Ru NPs. The obtained Ru NPs, predominantly in the Ru0 state with a Ru (100) lattice plane, were uniformly dispersed in the aqueous phase, exhibiting an average particle size of 2–3 nm. Ru@SLSaq displayed excellent catalytic activity for the hydrogenation of DPM and o-HDPM, achieving yields of 96.6% and 97.0% for DCHM and PHF, respectively, under mild conditions (n(substrate)/n(Ru) = 750, hydrogen pressure of 1.5 MPa, at 80 °C for 4 h). The calculated apparent activation energies (Ea) for the two reactions were found to be 46.5 kJ·mol–1 and 75.3 kJ·mol–1, respectively, and the catalytic system demonstrated good cycling stability. Experimental results, supported by DFT calculations, indicate that the complete hydrogenation processes of DPM and o-HDPM occur on the surface of Ru NPs via monophenyl ring adsorption, exhibiting small energy barrier differences across various pathways.
研究领域:
催化化学
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材料科学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Xiang Mei,Han Gao,Yang Ding,Chao Xue,Lijie Xu,Yong Wang,Lei Zhang,Mengyuan Ma,Zimiao Zhang,Yanyan Xiao,Xu Yang,Chengqi Yin,Zhan Wang,Mengmeng Yang,Dongyu Xia,Cai Wang
Membrane biofilm (MBf) technology is a promising biological water treatment process that combines membrane aeration with biofilms. To expand its application in the treatment of toxic organic wastewater, methane/air gas mixture-MBfs ((CH 4 + Air)-MBfs) and air-MBfs were coupled to enhance the treatment of p -nitroaniline (PNA) wastewater. Based on exploration of the membrane permeability of methane and oxygen, a hybrid MBf reactor was constructed, and the degradation characteristics of PNA and the coupling effects of (CH 4 + Air)-MBfs and air-MBfs were studied. The permeation flux of methane was found to be 1.114 g/(m 2 d) when using a methane/air gas mixture at an aeration pressure of 10 kPa, and this result was better than that when methane was used as the aeration gas alone. Aeration with a methane/air gas mixture provided conditions for realizing aerobic methane oxidation ; the aerobic methane oxidation that occurred in the (CH 4 + Air)-MBfs promoted the reduction of PNA, and the intermediates of PNA degradation were further degraded by the air-MBfs. At an influent PNA membrane area load of 1.67 g/(m 2 d), the PNA removal load reached 187.30 g/(m 3 d). The coupling of MBfs took advantage of different matrix-based MBfs and promoted the degradation of PNA by utilizing the synergistic effects of various functional microorganisms .
研究领域:
环境工程
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水处理技术
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生物过程
✓ 已验证
DOI
PubMed
高影响因子
Journal of Cleaner Production
·
2021
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IF 9.297
Junjie Li,Chunxing Li,Yanlin Li,Ruming Wang,Mingdian Zhou,Lixin Zhao,Xiaofang Pan,Guanjing Cai,Nan Lv,Jing Ning,Irini Angelidaki,Gefu Zhu
Conductive material assisted anaerobic digestion presented much interest and promising prospect in pollutant removal during wastewater treatment . The present study deeply investigated the effect iron/carbon in anaerobic digestion for dichlorophen (DCP) degradation and methane production in synthetic DCP wastewater treatment. Results showed that nano-zero valent iron/activated carbon (nZVI/AC) and zero valent iron/activated carbon (ZVI/AC) gave higher chemical oxygen demand (COD) conversion (42.18% and 42.61%) and DCP removal (98.49 wt% and 99.00 wt%) in acidification step with better methane production from anaerobic digestion of the pretreated effluent. Same phenomenon occurred in the direct anaerobic degradation process due to the formation of galvanic cells between iron and carbon. In comparison, applying iron/carbon in acidification as pretreatment strategy plus following effluent anaerobic degradation showed higher efficiency in methane production and DCP removal than that of direct anaerobic degradation. Specifically, the methane production was 253.70 mL and 253.41 mL in subsequent anaerobic digestion system after nZVI/AC and ZVI/AC acidification pre-treatment, which was higher than 224.37 mL and 246.31 mL in direct anaerobic digestion system. Microbial community analysis showed that Clostridium_sensu_stricto_1 was the dominated bacteria due to its important role in DCP wastewater treatment. Both acetoclastic and hydrogenotrophic methanogens were enhanced in iron/carbon added systems, which was also agreement with the strengthen in related genes involved in methanogenesis . In conclusion, the present work systematically investigated the enhancement role of iron/carbon system in anaerobic digestion for DCP wastewater treatment and paved way for future application.
研究领域:
环境工程
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污水处理
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微生物学
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厌氧生物技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Wenxin Fu,Yige Guo,Jianqiu Zhu,Xiaomin Zhang,Linjuan Zhang,Yuefeng Song,Guoxiong Wang,Xinhe Bao
Coupling the partial oxidation of methane (POM) to the anode of solid oxide electrolysis cells (SOECs) can significantly decrease the open-circuit voltage and electrical energy consumption of the SOECs. However, developing advanced anode for SOEC to selectively convert CH4 to syngas still remains a great challenge. Herein, we find that Ce substitution at the A-site of La0.5Ce0.5Fe0.5Ni0.5O3−δ can effectively alter the chemical state and coordination environment of Ni with the generation of NiO particles, and the air activation could further regulate the oxygen vacancy concentration and decrease the size of NiO particles, which both contribute to the enhanced POM performance with CH4 conversion of 45.20% and CO selectivity of 92.67% at 650 °C. Moreover, the introduction of POM to the anode could remarkably decrease the electrical energy consumption for CO production from 3.64 kWh m–3 of conventional SOECs to 0.86 kWh m–3 of CH4-assisted SOECs. This study provides an effective strategy for improving the electrochemical performance of CO2 electrolysis in SOECs while simultaneously converting CH4 to syngas at the anode.
研究领域:
材料科学
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能源工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2018
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IF 4.521
Ruiyi Wang,Zhiwei Wu,Zhikai Li,Zhangfeng Qin,Chengmeng Chen,Zhanfeng Zheng,Guofu Wang,Weibin Fan,Jianguo Wang
Polyoxymethylene dimethyl ethers (PODE n , with the formula of CH 3 O–(CH 2 O) n –CH 3 ), as a promising environmentally benign diesel fuel or additive with an enormous potential in the reduction of soot and NO x emissions, can be efficiently synthesized from methanol derivatives such as dimethoxymethane (DMM) and trioxymethylene (TOM), which requests a proper catalyst of high performance. In this work, the catalytic performance of graphene oxide (GO) in the synthesis of PODE n as well as its relation to the catalyst structure was thoroughly investigated. The results indicate that GO is an excellent catalyst in the synthesis of PODE n from DMM and TOM; a TOM conversion of 94.6% and selectivity of 86.0% to PODE 2–8 are achieved under mild reaction conditions, which is superior to the majority of the state-of-the-art catalysts. Meanwhile, the active species and characteristic layer structure of GO sheets catalytically responsible for PODE n formation were discriminated through selectively removing certain surface functional groups, thermally annealing at different temperatures, and carefully comparing with a series of model compounds. The results illustrate that the superior catalytic performance of GO in the PODE n synthesis should be ascribed to a synergy between the surface sulfonyl, hydroxyl and carboxyl groups present on the GO surface and the unique layered structure of GO sheets, wherein the surface sulfonyl groups act as the main active sites. The insights shown in this work are beneficial to a deep understanding on the catalytic principle of GO and development of efficient catalyst for the synthesis of PODE n .
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Zhi-Man Yang,Rong-Bo Guo,Xiao-Huan Dong
Using a batch anaerobic system constructed with 60 mL serum bottles, potential of a composite material with Fe 2 O 3 nanoparticles decorated on carbon nanotubes (CNTs) to enhance biomethane production was investigated. The composites (Fe 2 O 3 @CNTs) with well dispersed Fe 2 O 3 nanoparticles (4.5 nm) were fabricated by a facile thermal decomposition method in a muffle furnace under nitrogen atmosphere. Compared with Fe 2 O 3 , Fe 2 O 3 @CNTs showed a large specific surface area and good electrical conductivity. Supplementation of Fe 2 O 3 @CNTs to the propionate-degrading enrichments enhanced the methane production rate, which was 10.4-fold higher than that in the control experiment without material addition. The addition of Fe 2 O 3 @CNTs also not only showed a clearly electrochemical response to flavin and cytochrome C, but also reduced the electron transfer resistance when compared to the control. Comparative analysis showed that Fe 2 O 3 in Fe 2 O 3 @CNTs played a key role in initiating electrochemical response and triggering rapid methane production, while CNTs functioned as rapid electron conduits to facilitate electron transfer from iron-reducing bacteria (e.g., Acinetobacter , Syntrophomonas , and Geobacter ) to methanogens (e.g. Methanosarcina ).
研究领域:
环境工程
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微生物学
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能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chengxin Niu,Teng Cai,Xueqin Lu,Guangyin Zhen,Yang Pan,Xuan Ren,Xi Qin,Wanjiang Li,Yingxiang Tang,Zhongxiang Zhi
Underlying mechanism of continuous nano zero-valent iron (nZVI) supply in functional microbes enrichment and methane bioconversion of waste activated sludge were investigated in a lab-scale continuous stirred tank reactor (CSTR). Results indicated that methane productivity strongly relied on nZVI dosage ( R = 0.998, p (0.05) < 0.001) and leached Fe 2+ concentration ( R = 0.943, p (0.05) = 0.005). The higher nZVI dosage, the higher methane productivity and organic removal were achieved. The methane production rate reached 77.6 ± 9.7 mL/g-VS/d at 160 mg-nZVI/g-TS, increasing by 2.3 times than the phase without nZVI supply. The corrosion/dissociation of nZVI, except for serving as trace element and electron donors (H 2 /[H]), increased system buffering capacity (2835–3410 mg CaCO 3 /L), and decreased oxidation reduction potential from − 152 mV to − 240 mV. Such thermodynamically favorable environment facilitated the proliferation of organics-degrading bacteria ( Firmicutes , Chloroflexi , Smithella , etc.) and hydrogenotrophic methanogen ( Methanobacterium ). As a result, more large organic molecules such as proteins and polysaccharides were hydrolyzed into short-chain fatty acids, thus enhancing the methanogenesis. Furthermore, the continuous supply of nZVI regulated the colloidal properties of sludge flocs by altering particle size distribution and zeta potential via flocculation effect of the released Fe 2+ (136.4 ± 12.1 mg/L). The dewaterability of digested sludge was improved to a certain extent, with capillary suction time dropping to 84.8 ± 4.1 s. This study provided a more systematic understanding of the role of nZVI in promoting methane bioconversion and subsequent digested sludge dewatering and volume reduction, thus expanding the potential application of nZVI in real-world scenarios.
研究领域:
环境科学
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微生物学
✓ 已验证
DOI
高影响因子
Scientific Reports
·
2015
·Vol. 5
·期 1
·1-10
·
IF 5.578
Qiao Sen,Tian Tian,Qi Benyu,Zhou Jiti
This study presents a novel procedure for accelerating methanogenesis from wastewater by adding elemental manganese into the anaerobic digestion system. The results indicated that elemental manganese effectively enhanced both the methane yield and the production rate. Compared to the control test without elemental manganese, the total methane yield and production rate with 4 g/L manganese addition increased 3.4-fold (from 0.89 ± 0.03 to 2.99 ± 0.37 M/gVSS within 120 h) and 4.4-fold (from 6.2 ± 0.1 to 27.2 ± 2.2 mM/gVSS/h), respectively. Besides, more acetate consumption and less propionate generation were observed during the methanogenesis with manganese. Further studies demonstrated that the elemental manganese served as electron donors for the methanogenesis from carbon dioxide and the final proportion of methane in the total generated gas with 4 g/L manganese addition reached 96.9%, which was 2.1-fold than that of the control (46.6%).
研究领域:
环境工程
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生物技术
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微生物学
✓ 已验证
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2020
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IF 2.627
Shenglai Li,Lisong Fan,Lina Song,Dangguo Cheng,Fengqiu Chen
Iron-containing zeolites play an important role in the selective oxidation of methane to oxygenates by nitrous oxide. A solid-state ion exchange method is adopted to prepare Fe-MOR zeolite catalysts with different amounts of extra-framework Al. EPR spectra and UV–vis spectra show that the percentage of iron ions in tetrahedral or octahedral coordination increases while those of clustered Fe species decrease by the addition of extra-framework Al species. Nitrous oxide titration reveals that more active Fe centers are formed, which promote the nitrous oxide consumption. The number of active centers in the catalyst with the introduction of extra-framework Al is about four times that of the catalyst without the addition of extra-framework Al. Due to this, there is an increase in the methane conversion, total selectivity and yield of oxygenates.
研究领域:
化学
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催化作用
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）