GEOCHIMICA ET COSMOCHIMICA ACTA
·
2021
·
IF 5.01
Zhiyong Lin,Xiaoming Sun,Harald Strauss,Sümeyya Eroglu,Michael E. Böttcher,Yang Lu,Jinqiang Liang,Jie Li,Jörn Peckmann
Methane seepage causes significant changes in the local diagenetic environment and impacts the marine sedimentary cycles of sulfur, carbon, and molybdenum (Mo), which are intimately linked to each other. Molybdenum isotopic compositions were determined for authigenic carbonate nodules and bulk sediments of a 230-m long sediment core collected at a methane seep site in the South China Sea. Authigenic carbonate nodules occur at different sediment depths and display low δ 13 C values around −50‰ revealing that carbon predominantly derived from biogenic methane. Moreover, seep carbonate nodules are substantially enriched in Mo (Al-normalized enrichment factors Mo EF between 27 and 70), and display nearly constant δ 98 Mo values around an average of +1.9‰ (relative to NIST3134 = +0.25‰), close to the Mo isotopic composition of modern seawater (+2.3‰). Linear positive correlations between δ 98 Mo values and pyrite sulfur contents and Mo contents were identified for seep carbonate samples. This implies that Mo scavenging into pyrite is likely controlled by hydrogen sulfide availability derived from sulfate-driven anaerobic oxidation of methane (SD-AOM). The essentially constant and high δ 98 Mo values suggest that Mo species were nearly quantitatively incorporated into the authigenic carbonates under highly sulfidic conditions, probably at times when the sulfate-methane transition zones (SMTZ) was situated at shallow sediment depth at times of high seepage activity. In contrast, bulk sediments that exhibit typical marine δ 13 C values close to 0‰ (versus VPDB), hence devoid of methane-derived seep carbonates, are characterized by low Mo contents (Mo EF = ~0.9). Their lower δ 98 Mo values mostly ranging from +0.2 to +0.8‰, in accord with low Mo contents, likely reflect input of detrital Mo. Bulk sediments bearing seep carbonate nodules display variable δ 13 C values lower than −5‰ and are characterized by a wide range in Mo contents (Mo EF from 1.5 to 45.3) and δ 98 Mo values (+0.7 to +3.0‰). The high δ 98 Mo values of some sediment samples, relative to the seep carbonate signature, might indicate an additional accumulation of a 98 Mo enriched pool of molybdenum during later SD-AOM at a deeper SMTZ postdating initial seep carbonate formation; such 98 Mo enrichment was probably caused by preceding preferential removal of lighter Mo isotopes from pore fluids. Our results indicate that Mo isotope systematics of seep deposits can provide constraints on the dynamics of the biogeochemical cycling of carbon, sulfur, and trace elements in methane seep environments. A potential for authigenic carbonates to archive the Mo isotopic composition of seawater is indicated, but will have to be assessed in future studies.
研究领域:
海洋学
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地球化学
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产品关联
DOI
高影响因子
Sustainable Chemistry and Pharmacy
·
2020
·
IF 3.294
Wenfeng Zhao,Hu Li,Yan Li,Jingxuan Long,Yufei Xu,Song Yang
Using CO 2 as a low-cost C1 resource to produce value-add products was considered as a promising strategy for the sustainable carbon cycle . Herein, a base-promoted reductive functionalization of CO 2 and 1,2-phenylenediamine for the synthesis of benzimidazole was developed using hydrosilane as an H-donor. Commercially available acetate salt CH 3 COOK used as a budget catalyst could furnish various benzimidazoles with moderate to excellent yields (42-95%) under mild conditions (40 °C, 1 bar CO 2 ). The reaction mechanism undergoing cascade N -formylation, cyclization, and reduction was preliminarily confirmed by attenuated total reflection (ATR) technique and control experiments.
研究领域:
有机化学
·
绿色化学
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DOI
高影响因子
ENERGY & FUELS
·
2024
·
IF 5.2
Yue Zhang,Jing-Chun Feng,Yuhang Zhang,Bin Wang,Jinyi Liu,Yi Wang,Si Zhang
On the cold seep seafloor, methane hydrate is an important form of carbon storage. The stability of methane hydrates and mechanisms of ionic effects on hydrates are closely related to seafloor methane release and carbon cycling. Cold seeps are endowed with abundant and high-quality hydrate resources under the environmental conditions of low temperatures and high pressures. Methane hydrates are seen as a potential source of renewable energy and a possible form of energy storage, as the global demand for clean energy increases. Although studies have focused on the formation and dissociation processes of methane hydrates, the influence of seawater ions on the kinetics of hydrate formation is still unclear. In this study, we studied the formation kinetics of methane hydrate in ion systems, analyzed the effects of various main ions, and compared them with in situ seawater composition. The phase equilibrium point of methane hydrate in the in situ seawater system was experimentally determined by us to better understand the stability. The degree of inhibition on the methane hydrate formation kinetics in natural seawater is more closely to that of CaCl2, MgCl2, and SrCl2, as indicated by gas consumption during methane hydrate formation. However, NaCl exhibits a greater inhibition effect than that of CaCl2, MgCl2, and SrCl2. The thermodynamic behavior of in situ seawater is consistent with the inhibition degree of SrCl2 on methane hydrate formation. In addition, morphological characteristics of hydrates possessed dense powdery particles and ice particles on the surface of the seawater–methane system, which combined with both hydrate morphologies, the pure water–methane system (ice particles), and the saline ions–methane system (powdery particles). The findings of this study may provide a reference for further exploration of methane hydrate formation in cold seep environments and provide a basis for an in-depth understanding of submarine methane release and carbon cycling.
研究领域:
海洋科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2020
·
IF 5.647
Jia Liu,Jan Baeyens,Yimin Deng,Tianwei Tan,Huili Zhang
The abatement of CO 2 emitted from combustion is a hot research topic. Current CO 2 capture techniques of adsorption, absorption, membrane separation and cryogenics involve high investment and operation costs. For moderate and high temperature exhaust gas, carbonation/decarbonation cycles offer an attractive alternative. An objective assessment method (screening index) was applied to select the most appropriate chemical reactions, with MgO and Mg(OH) 2 being screened as having the highest potential. Macro-thermogravimetric experiments determined a CO 2 capture yield between 60 and 70% for Mg(OH) 2 at temperatures between 260 and 330 °C, and from 85 to 98% for MgO at temperatures of 400–440 °C. Reaction rates were measured for both MgO–CO 2 and Mg(OH) 2 –CO 2 . The reaction kinetics are best fitted by the Jander 3D-diffusion approach. The Arrhenius equation is applied to the reaction rate constant, and both its activation energy and pre-exponential factor are determined. Integrating the Jander expression in the reaction rate equation enables to predict the CO 2 -capture conversion for any selected temperature and/or contact time.
研究领域:
化学工程
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环境科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Bio Materials
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2020
·
IF 0
Xinke Kong,Panpan Gai,Feng Li
Biohybrid photoelectrochemical systems could combine the light-harvesting ability of semiconductor photocatalysts and the CO2-processing capability of biocatalysts to realize CO2 reduction. How to develop the energy-utilized model can be of importance for the mechanism exploration of photosynthesis. Here, a biohybrid photoelectrochemical system based on HCOO––CO2 circulation was developed to realize the conversion both of solar-to-electric energy and chemical-to-electric energy. The device consists of a TiO2 nanoparticle photoanode and a laser-scribed graphene/formate dehydrogenase biocathode, which was utilized for the formic acid oxidation and the biocatalysis reduction of CO2 to HCOO–, respectively. The as-proposed biohybrid photoelectrochemical system exhibits good performance with an open-circuit potential of 0.93 V and a maximum power output density of 76 μW cm–2. This ingenious strategy not only exploits a robust carbon circulation system for the conversion of solar energy but also provides a way of constructing complex artificial photosynthesis systems.
研究领域:
生物技术
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能源科学
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环境科学
✓ 已验证
DOI
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Donglai Pan,Yongjie Wang,Ying Tao,Chi Zhang,Kangning Xu,Hong Li,Guisheng Li,Hexing Li
The artificial photosynthesis system is expected to achieve efficient solar energy conversion and artificial carbon recycling. Here, a dual-photoelectrode artificial photosynthesis system is constructed by integrating Cu-p-Si NWs photocathode and FeNiO x /WO 3 /W photoanode, enabling efficient carbon dioxide reduction (CO 2 RR) and oxygen evolution reaction (OER). In the cathodic reaction, the photocathode exhibits the enhanced CO 2 RR performance under visible light irradiation, where the CO Faradaic efficiency is two times higher than the dark condition at −1.05 V vs. RHE. Syngas (CO and H 2 ) is obtained with a CO/H 2 ratio of 1:2. In the anodic reaction, the FeNiO x modified WO 3 /W photoanode displays a lower potential of 2.47 V vs. RHE at 10 mA/cm 2 compared to WO 3 /W photoanode. Moreover, the FeNiO x /WO 3 /W|Cu-p-Si NWs system exhibits a significantly reduced cell voltage at 10 mA/cm 2 . The modification with FeNiO x effectively improves the efficiency of the overall cell reaction by accelerating the sluggish OER kinetics. This work provides a feasible strategy for carbon recycling through the well-designed dual-photoelectrode artificial photosynthesis system.
研究领域:
能源科学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2024
·Vol. 121
·期 45
·e2413245121
·
IF 9.4
Lu Wang,Da Lin,Ke-Qing Xiao,Li-Juan Ma,Yan-Mei Fu,Yu-Xin Huo,Yanjie Liu,Mao Ye,Ming-Ming Sun,Dong Zhu,Matthias C. Rillig,Yong-Guan Zhu
Microplastic is globally regarded as an important factor impacting biogeochemical cycles, yet our understanding of such influences is limited by the uncertainties of intricate microbial processes. By multiomics analysis, coupled with soil chemodiversity characterization and microbial carbon use efficiency (CUE), we investigated how microbial responses to microplastics impacted soil carbon cycling in a long-term field experiment. We showed that biodegradable microplastics promoted soil organic carbon accrual by an average of 2.47%, while nondegradable microplastics inhibited it by 17.4%, as a consequence of the virus–bacteria coadaptations to the microplastics disturbance. In the relevant functional pathways, nondegradable microplastics significantly (P < 0.05) enhanced the abundance and transcriptional activity related to complex carbohydrate metabolism, whereas biodegradable microplastics significantly (P < 0.05) promoted functions involved in amino acid metabolism and glycolysis. Accordingly, viral lysis enhanced in nondegradable microplastics treatments to introduce more complex organic compounds to soil dissolved organic matters, thus benefiting the oligotrophs with high carbon metabolic capabilities in exploitation competition. In contrast, biodegradable microplastics enriched viral auxiliary metabolic genes of carbon metabolism through “piggyback-the-winner” strategy, conferring to dominant copiotrophs, enhanced substrate utilization capabilities. These virus–host interactions were also demonstrated in the corresponding soil plastisphere, which would alter microbial resource allocation and metabolism via CUE, affecting carbon storage consequently. Overall, our results underscore the importance of viral–host interactions in understanding the microplastics-dependent carbon storage in the soil ecosystem.
研究领域:
生态学
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环境科学
·
微生物学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jiangyong Yuan,Chunqiang Lu,Zhenhua Gu,Jun Cai,Han Zhao,Danyang Li,Lei Jiang,Haiwen Xu,Zhi qiang Li,Kongzhai Li
Carbon cycling, instead of conventional oxygen cycling in chemical looping, overcomes the limitations of oxygen storage capacity of oxygen carriers and enables the reaction to proceed under relatively mild conditions. In this study, we designed a high-performance carbon-storage catalyst (Ni-Co/Al 2 O 3 ) for chemical looping conversion of CH 4 and CO 2 to H 2 and CO. The physico-chemical characterizations suggested that the Co alloyed with Ni could result in larger active metal particles and simultaneously benefit the bending of carbon deposits toward the periphery of the active sites, avoiding the quick deactivation of catalysts due to the encapsulation of the active sites by carbon deposits and generating a higher carbon capacity (23.59 vs. 14.08 mol/kg). In addition, the alloying of Co with Ni could weaken the graphitization of carbon deposits, thus facilitating the carbon elimination and catalyst regeneration in the CO 2 conversion step, strongly improving the cycling stability during long-term testing.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Zhaojiang Liu,Jiayang Hu,Yanjun Li,Yong Yu
Herbicide acetochlor (ACT) is widely used in agricultural production, but it remains unclear whether microplastics (MPs) from agricultural films exacerbate its harmful effects on soil health. Here, a microcosm cultivation experiment was conducted to investigate the impacts of PE (Polyethylene)-MPs and PBAT (polybutylene adipate terephthalate)-MPs with ACT (MPs/ACT) on soil health. Results showed that MPs/ACT treatment caused soil acidification, depletion of organic carbon and ammonium, altered enzyme activities, and influenced greenhouse gas emissions compared to ACT alone. MPs/ACT co-exposure also restructured microbial communities, reducing alpha diversity, increasing co-occurrence network complexity, enriching putative contaminant degraders, and enhancing the relative abundance of key nitrogen-cycling genes, enzymes, and carbon-cycling genes. Notably, PBAT/ACT stimulated nitrification-denitrification processes more than PE/ACT, indicating polymer-specific effects on soil nutrient cycling. Overall, MPs/ACT decreased soil health by 8.89 % - 14.63 %, greater than 8.39 % caused by ACT alone. These results demonstrate that MPs exacerbate the toxic effects of ACT on soil health. Mitigation strategies, such as reducing MP inputs, optimizing herbicide use, and incorporating biochar or microbial amendments, may help to restore soil health and maintain ecosystem stability. This study provides critical insights into the compounded impacts of MPs and herbicides on soil ecosystems.
研究领域:
环境科学
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土壤生物学
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农业生态学
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环境污染与修复
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微生物生态学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 33
·27546-27556
·
IF 9.5
Changhu Leng,Huijie Li,Qianfeng Zhou,Chenyang Ma,Yongchao Wang,Shengdong Zhang,Chuanya Li,Wanglei Wang,Zhi-Jun Li
Catalytic upcycling of polyolefin (PO) waste into liquid fuels represents a promising strategy for closing the carbon loop but remains challenged by the reliance on noble-metal catalysts and the generation of low-value gaseous byproducts. Here we report a non-noble metal bifunctional catalyst, Ni–W/ZrO2, featuring Ni metal sites for (de)hydrogenation and WOx acid sites for C–C bond cleavage and isomerization. The catalyst enables complete conversion of low-density polyethylene (LDPE, Mw = 96.4 kDa, Đ = 4.6) under mild conditions (250 °C, 3 MPa H2) within 10 h, affording a high liquid fuel yield of 75.6 wt%. The liquid products are dominated by branched alkanes (C5–C20) with a branching index of 85.6%, affording a high research octane number of 88.9, which is comparable to that of commercial gasoline (86.6). Compared to existing non-noble metal systems, Ni–W/ZrO2 exhibits superior catalytic activity and effectively suppresses methane formation. Mechanistic analyses reveal the generation of partially electropositive Ni species that promote C–H bond activation. The catalyst also demonstrates excellent durability over five consecutive cycles and broad compatibility with various polyolefin wastes, providing a cost-effective and scalable strategy for sustainable plastic waste valorization.
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产品关联
DOI
高影响因子
Small Methods
·
2024
·
IF 10.7
Yajuan Niu,Qinbo Liu,Xu Ou,Yingjie Zhou,Zhe Sun,Feng Yan
Large amounts of small molecule dyes leak into the ecosystems annually in harmful and unsustainable ways. Polymer dyes have attracted much attention because of their high migration resistance, excellent stability, and minimized leakage. However, the complex synthesis process, high cost, and poor degradability hinder their widespread application. Herein, green and sustainable polymer dyes are prepared using natural dye quercetin (Qc) and CO 2 through a one-step process. The CO 2 -sourced polymer dyes show strong migration resistance, high stability, and can be degraded on demand. Additionally, the CO 2 -sourced polymer dyes showed unique responses to Zn 2+ , leading to significantly enhanced fluorescence, highlighting their potential for information encryption/decryption. The CO 2 -sourced polymer dyes can solve the environmental hazards caused by small molecule dye leakage and promote the carbon cycle process. Meanwhile, the one-step synthesis process is expected to achieve sustainable and widespread utilization of CO 2 -sourced polymer dyes.
研究领域:
材料科学
·
环境科学
·
化学
·
可持续性
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Jie Wang,Andrew J. Tanentzap,Yuanze Sun,Jia Shi,Jianguo Tao,Xiang Wang,Li Xu,Jia Ding,Bing Feng,Jing Gao,Dayi Zhang,Xiaofeng Cao
Microbial regulation of soil carbon sequestration is vulnerable to anthropogenic stressors, notably microplastic pollution. Microplastics can release carbon-based compounds that serve as potential substrates for soil heterotrophic microbes. The impact of this novel microplastic-derived dissolved organic matter (MP-DOM) on soil carbon cycling and the underlying mechanisms remain largely unexplored. Here, short-term soil microcosm experiments were conducted with MP-DOM sourced from pristine and aged microplastics to compare their effects on soil carbon respiration against natural dissolved organic matter (NOM). The underlying mechanisms are investigated by estimating the spectroscopic and molecular signatures of MP-DOM and NOM, and comparing their effects on soil microbial physiological properties. Our findings reveal that MP-DOM leads to 36.9–42.3% higher CO2 emissions from soils than NOM, attributed to its greater bioavailability. MP-DOM simultaneously stimulates greater microbial quantity, phenotypic activities, and carbon utilization efficiency because this carbon is more biochemically accessible than NOM. Network analysis indicates stronger interconnections among labile molecules and bacterial taxa in MP-DOM treatments compared to NOM-treated soils, suggesting enhanced microbial capacity to utilize the more readily available MP-DOM. This study demonstrates that MP-DOM accelerates soil microbial respiration by mediating their physiological traits, with potential implications for climate change.
研究领域:
环境科学
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土壤微生物学
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生物地球化学
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气候变化
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生态毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）