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Enhanced CO 2 photoreduction to CH 4 via *COOH and *CHO intermediates stabilization by synergistic effect of implanted P and S vacancy in thin-film SnS 2

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Nano Energy 2024年 128卷

作者： Tadios Tesfaye Mamo Mohammad Qorbani Adane Gebresilassie Hailemariam Raghunath Putikam Che-Men Chu Ting-Rong Ko Amr Sabbah Chih-Yang Huang Septia Kholimatussadiah Tadesse Billo Mahmoud Kamal Hussien Shuo-Yun Chang Ming-Chang Lin Wei-Yen Woon Heng-Liang Wu Ken-Tsung Wong Li-Chyong Chen Kuei-Hsien Chen Department of Chemistry National Taiwan University Taipei 10617 Taiwan Institute of Atomic and Molecular Sciences Academia Sinica Taipei 10617 Taiwan Nano Science and Technology Program Taiwan International Graduate Program Academia Sinica Taipei 11529 Taiwan Institute of Physics Academia Sinica Taipei 11529 Taiwan Center for Condensed Matter Sciences National Taiwan University Taipei 10617 Taiwan Center of Atomic Initiative for New Materials National Taiwan University Taipei 10617 Taiwan Sustainable Chemical Science and Technology Program Taiwan International Graduate Program Academia Sinica Taipei 11529 Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu 30010 Taiwan Institute of Chemistry Academia Sinica Taipei 11529 Taiwan Department of Chemistry College of Natural Science Dire Dawa University Dire Dawa 1362 Ethiopia Department of Physics National Central University Jungli 32054 Taiwan Tabbin Institute for Metallurgical Studies Tabbin Helwan 109 Cairo 11421 Egypt International Graduate Program of Molecular Science and Technology National Taiwan University Taipei 10617 Taiwan Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Taipei 11529 Taiwan Department of Physics National Taiwan University Taipei 10617 Taiwan Materials Science Division Argonne National Laboratory 9700 S. Cass Avenue Lemont IL 60439 United States Department of Chemistry Faculty of Science Assiut University Assiut 71516 Egypt Department of Chemistry National Taiwan Normal University Taipei 10610 Taiwan National Synchrotron Radiation Research Center Hsinchu 30092 Taiwan

Reduction of CO 2 to value-added hydrocarbons through artificial photosynthesis is one of the way to address the energy crisis and climate change issues. It is known that lowering the activation energy of CO 2 molecules on the photocatalyst surface and key intermediates is crucial in photocatalytic CO 2 reduction. Herein, we present phosphorus-implanted 20-nm SnS 2 continuous thin film with sulfur vacancies ( i.e. , S V -SnS 2 :P where P substitutes on S sites). The fabrication process involves thermal evaporation, post-sulfurization, and ion implantation. Our gas-phase photocatalytic experiments show an enhanced and selective CO 2 photoreduction to CH 4 with a yield of 0.13 µmol cm −2 and selectivity of 92 % under solar-light irradiation for 4 h over an optimal ∼4.5 % P and ∼16 % S V . Experimental observations, conducted through X-ray absorption near edge, in situ near ambient pressure X-ray photoelectron, and in situ Fourier transform infrared spectroscopies, along with first-principle density functional theory calculations. Results reveal that P dopant is significantly affected by nearby S V via local charge density transfer from P to the nearest Sn and next-nearest S neighbor atoms, consequently, leads to the stabilization of *COOH and *CHO intermediates, where asterisks stand for P as the active site. Our results demonstrate how active site modulation, without using precious co-catalysts, plays a crucial role in intermediate stabilization in a wireless photocatalysis process.

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Elongated Sn-Doped G-C3n4 as a Novel Photoelectrocatalyst for Water Oxidation

SSRN

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SSRN 2022年

作者： Revaprasadu, Neerish Aboubakr, Ahmed Esmail A. El Rouby, Waleed M.A. Khan, Malik Dilshad Hung, Chen-Hsiung Millet, Pierre Sustainable Chemical Science and Technology Taiwan International Graduate Program Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu30010 Taiwan Institute of Chemistry Academia Sinica 128 Sec 2 Academia Rd. Nankang Taipei11529 Taiwan Beni-Suef University Beni-Suef62511 Egypt Department of Chemistry University of Zululand Private Bag X1001 Kwadlangezwa3886 South Africa Institute of Physical Chemistry Polish Academy of Sciences Kasprzaka 44/52 Warsaw01-224 Poland Paris-Saclay University ICMMO-Eríee UMR CNRS 8182 Orsay91405 France

The photocatalytic performance of graphitic carbon nitride can be enhanced multifold by introducing suitable dopants. Here we report the incorporation of a cost-effective, non-toxic and abundant element, i.e., tin, in one-dimensional semiconducting carbon nitride (1D-g-C3N4). Various samples with different tin doping concentrations were prepared. A novel procedure was used to introduce varying amounts of tin to the 1D- g-C3N4 framework. The new photocatalysts (Sn-1D-g-C3N4) were characterized by p-XRD and FT-IR measurements, confirming the absence of tin oxide and the formation of tin-nitrogen bonds involving the 1D-g-C3N4 backbone. The SEM, EDX, and XPS measurements demonstrated the longitudinal morphology and the presence of tin in the hybrids. BET measurements showed a relative increase in the specific surface area for the composites. The optical measurements showed enhanced solar light absorption and promoted charge carriers’ separation after insertion of Sn to1D-g-C3N4. Photoelectrochemical water dissociation measurements showed that 10% tin doping increased the activity of 1D-g-C3N4 to water photo-oxidation about four times. This improvement was analyzed by electrochemical impedance spectroscopy measurements. © 2022, The Authors. All rights reserved.

关键词： Light absorption

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Alloying behavior of wide band gap alkaline-earth chalcogenides

arXiv

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arXiv 2020年

作者： Millican, Samantha L. Clary, Jacob M. Bartel, Christopher J. Singstock, Nicholas R. Holder, Aaron M. Musgrave, Charles B. Department of Chemical and Biological Engineering University of Colorado BoulderCO80309 United States Materials and Chemical Science and Technology Center National Renewable Energy Laboratory GoldenCO80401 United States Renewable and Sustainable Energy Institute University of Colorado Boulder BoulderCO80309 United States Materials Science and Engineering Program University of Colorado Boulder BoulderCO80309 United States

Alloying is a powerful tool for tuning materials that facilitates the targeted design of desirable properties for a variety of applications. In this work, we provide a comprehensive investigation of the synthetic accessibility and electronic properties of nine alkaline-earth chalcogenide anion alloys (CaS1-xOx, CaS1-xSex, CaS1-xTex, SrS1-xOx, SrS1-xSex, SrS1-xTex, MgS1-xOx, MgS1-xSex, and MgS1-xTex). We show that isostructural alloying within the rock salt structure is favored for all systems except MgS1-xTex, which is predicted to be a heterostructural alloy between the rock salt and wurtzite structures. Alloys of S and Se are shown to be readily accessible for all cations with low miscibility critical temperatures, enabling continuous tuning of electronic properties across this composition space. Alloys of S and Te have higher critical temperatures but may be accessible through non-equilibrium synthesis strategies and are predicted here to have desirable electronic properties for optoelectronics with wide band gaps and lower effective masses than alloys of S and Se. Anion alloying in MgS1-xTex stabilizes the wurtzite structure across a significant fraction of composition space, which may make it of particular interest as a transparent conducting material due to its lower effective masses and a higher band gap than the rock salt structure. Zero-point corrected random phase approximation (RPA) energies were computed to resolve the small polymorph energy differences of the Mg compounds and are shown to be critical for accurately describing the thermodynamic properties of the corresponding alloys. Copyright © 2020, The Authors. All rights reserved.

关键词： Electronic properties

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Sn-Doped G-C3n4 as a Novel Photoelectrocatalyst for Water Oxidation

SSRN

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SSRN 2022年

作者： Aboubakr, Ahmed Esmail A. Khan, Malik Dilshad Revaprasadu, Neerish Millet, Pierre Hung, Chen-Hsiung El Rouby, Waleed M.A. Sustainable Chemical Science and Technology Taiwan International Graduate Program Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu30010 Taiwan Institute of Chemistry Academia Sinica 128 Sec 2 Academia Rd. Nankang Taipei11529 Taiwan Beni-Suef University Beni-Suef62511 Egypt Department of Chemistry University of Zululand Private Bag X1001 Kwadlangezwa3886 South Africa Institute of Physical Chemistry Polish Academy of Sciences Kasprzaka 44/52 Warsaw01-224 Poland Paris-Saclay University ICMMO-Eríee UMR CNRS 8182 Orsay91405 France

The photocatalytic performance of graphitic carbon nitride can be enhanced multifold by introducing suitable dopants. Here we report the incorporation of a cost-effective, non-toxic and abundant element, i.e., tin, in elongated semiconducting carbon nitride (g-C3N4). Various samples with different tin doping concentrations were prepared. A novel procedure was used to introduce varying amounts of tin to the g-C3N4 framework. The new photocatalysts (Sn-g-C3N4) were characterized by X-Ray Diffraction (XRD) and FT-IR measurements, confirming the absence of tin oxide and the formation of tin-nitrogen bonds involving the g-C3N4 backbone. The SEM, EDX, TEM and XPS measurements demonstrated the longitudinal morphology and the presence of tin in the hybrids. BET measurements showed a relative increase in the specific surface area for the composites. The optical measurements showed enhanced solar light absorption and promoted charge carriers’ separation after insertion of Sn to g-C3N4. Photoelectrochemical water dissociation measurements showed that 10% tin doping increased the activity of g-C3N4 to water photo-oxidation about four times. This improvement was analyzed by electrochemical impedance spectroscopy measurements. © 2022, The Authors. All rights reserved.

关键词： Morphology

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Enhanced exopolysaccharide production of Cordyceps militaris via mycelial cell immobilization on plastic composite support in repeated-batch fermentation

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International Journal of Biological Macromolecules 2023年第1期250卷 126267页

作者： Lin, Shin-Ping Sung, Ting-Hsuan Angkawijaya, Artik Elisa Go, Alchris Woo Hsieh, Chang-Wei Hsu, Hsien-Yi Santoso, Shella Permatasari Cheng, Kuan-Chen School of Food Safety Taipei Medical University #250 Wuxing Street Xinyi Dist. Taipei11042 Taiwan Research Center of Biomedical Device Taipei Medical University #250 Wu-Hsing Street Taipei11031 Taiwan TMU Research Center for Digestive Medicine Taipei Medical University #250 Wu-Hsing Street Taipei11031 Taiwan Ph.D. Program in Drug Discovery and Development Industry Taipei Medical University #250 Wu-Hsing Street Taipei11031 Taiwan Taiwan Institute of Food Science and Technology National Taiwan University #1 Sec. 4 Roosevelt Rd. Taipei10617 Taiwan Institute of Food Science and Technology National Taiwan University #1 Sec. 4 Roosevelt Rd. Taipei10617 Taiwan School of Nutrition and Health Sciences Taipei Medical University #250 Wu-Hsing Street Taipei11031 Taiwan Center for Sustainable Resource Science RIKEN Yokohama230-0045 Japan Department of Chemical Engineering National Taiwan University of Science and Technology #43 Sec. 4 Keelung Rd Taipei10607 Taiwan Department of Food Science and Biotechnology National Chung Hsing University South Dist. Taichung City40227 Taiwan Department of Medical Research China Medical University Hospital North Dist. Taichung City404333 Taiwan Taiwan Institute of Biotechnology National Taiwan University #1 Sec. 4 Roosevelt Rd. Taipei10617 Taiwan School of Energy and Environment Department of Materials Science and Engineering City University of Hong Kong Kowloon Tong Hong Kong Shenzhen Research Institute of City University of Hong Kong Shenzhen518057 China Department of Chemical Engineering Widya Mandala Surabaya Catholic University Kalijudan 37 Surabaya60114 Indonesia Collaborative Research Center for Zero Waste and Sustainability Jl. Kalijudan 37 East Java Surabaya60114 Indonesia Institute of Biotechnology National Taiwan University #1 Sec. 4 Roosevelt Rd. Taipei10617 Taiwan Department of Medical Research China Medical University Hospital China Medical University 91 Hsueh-Shih Road Taichung40

Repeated-batch fermentation with fungal mycelia immobilized in plastic composite support (PCS) eliminates the lag phase during fermentation and improves metabolite productivity. The strategy is implemented herein, and a novel modified PCS is developed to enhance exopolysaccharide (EPS) production from the medicinal fungus Cordyceps militaris. A modified PCS (SYE + PCS) was made by compositing polypropylene (PP) with a nutrient mixture containing soybean hull, peptone, yeast extract, and minerals (SYE+). The use of SYE + PCS has consistent cell productivity throughout the multiple fermentation cycles, which resulted in a more higher cell productivity after second batch compared to unmodified PCS. The cell grown on SYE + PCS also generates a higher yield of EPS (3.36, 6.93, and 5.72 g/L in the first, second, and third fermentation cycles, respectively) up to three-fold higher than the cell immobilized on unmodified PCS. It is also worth noting that the EPS from mycelium grown on SYE + PCS contains up to 2.3-fold higher cordycepin than those on unmodified PCS. The presence of nutrients in SYE + PCS also affects the hydrophobicity and surface roughness of the PC, improving mycelial cell adhesion. This study also provides a preliminary antioxidant activity assessment of EPS from immobilized C. militaris grown with SYE + PCS. © 2023

关键词： Mycelium

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Improvement of extracellular polysaccharides production from Cordyceps militaris immobilized alginate beads in repeated-batch fermentation

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LWT 2024年 193卷

作者： Hou, Shi-Jing Cheng, Kuan-Chen Lin, Shyh-Hsiang Hsiao, I-Lun Santoso, Shella Permatasari Singajaya, Stephanie Chou, Yu-Chieh Lin, Shin-Ping Master Program in Food Safety Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan Institute of Biotechnology National Taiwan University 1 Roosevelt Rd. Sec. 4 Taipei10617 Taiwan Graduate Institute of Food Science and Technology National Taiwan University 1 Roosevelt Rd. Sec. 4 Taipei10617 Taiwan Department of Medical Research China Medical University Hospital China Medical University 91 Hsueh-Shih Rd. Taichung40402 Taiwan Department of Optometry Asia University 500 Lioufeng Rd. Wufeng Taichung41354 Taiwan School of Nutrition and Health Sciences Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan School of Food Safety Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan Department of Chemical Engineering Widya Mandala Surabaya Catholic University Kalijudan 37 East Java Surabaya60114 Indonesia Collaborative Research Center for Sustainable and Zero Waste Industries Kalijudan 37 East Java Surabaya60114 Indonesia Ph.D. Program in Drug Discovery and Development Industry Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan Research Center of Biomedical Device Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan TMU Research Center for Digestive Medicine Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan

Cordyceps militaris (C. militaris) is a unique medicinal fungus of the genus Cordyceps. It has high economic value due to various biological functions from the extracellular polysaccharides (EPSs) it produces. The aim of this study was to establish a mycelium-immobilization system for EPS production in a bubble column system. First, EPS production was optimized by 90.2% (from 0.72 to 1.37 g/L) using response surface methodology under an alginate-immobilized mycelium system with 6 days of cultivation. The highest EPS production was obtained (5.3 g/L) in a flask system through elongation to 15 days of cultivation. EPS production subsequently further increased to 10.42 g/L utilizing a bubble column reactor. Furthermore, the system can be reused for at least three rounds. In the EPS characteristics analysis, the produced EPSs were mainly composed of glucose and galactose. They presented strong antibacterial activity against Staphylococcus aureus. In terms of antioxidant activity, respective the EPS concentration that caused 50% scavenging of DPPH and ABTS free radicals values (IC50) were 4.65 and 7.92 mg/mL. In summary, these findings should be helpful for establishing a suitable industrial fermentation system for C. militaris and can be studied in the food and medical industries in future work. © 2024 The Authors

关键词： Mycelium

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Biological evaluation of sulfonate and sulfate analogues of lithocholic acid: A bioisosterism-guided approach towards the discovery of potential sialyltransferase inhibitors for antimetastatic study

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Bioorganic & medicinal chemistry letters 2024年 105卷 129760页

作者： Ser John Lynon P Perez Chia-Ling Chen Tzu-Ting Chang Wen-Shan Li Institute of Chemistry Academia Sinica Taipei 115 Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu 300 Taiwan Sustainable Chemical Science and Technology Taiwan International Graduate Program Academia Sinica Taipei 115 Taiwan Biomedical Translation Research Center Academia Sinica Taipei 115 Taiwan. Institute of Chemistry Academia Sinica Taipei 115 Taiwan. Biomedical Translation Research Center Academia Sinica Taipei 115 Taiwan Department of Medicinal and Applied Chemistry College of Life Science Kaohsiung Medical University Kaohsiung 807 Taiwan Ph.D. Program in Drug Discovery and Development Industry College of Pharmacy Taipei Medical University Doctoral Degree Program in Marine Biotechnology National Sun Yat-Sen University Kaohsiung 804 Taiwan Department of Chemistry College of Science Tamkang University New Taipei City 251 Taiwan. Electronic address: wenshan@gate.sinica.edu.tw.

The naturally occurring bile acid lithocholic acid (LCA) has been a crucial core structure for many non-sugar-containing sialyltranferase (ST) inhibitors documented in literature. With the aim of elucidating the impact of the terminal carboxyl acid substituent of LCA on its ST inhibition, in this present study, we report the (bio)isosteric replacement-based design and synthesis of sulfonate and sulfate analogues of LCA. Among these compounds, the sulfate analogue SPP-002 was found to selectively inhibit N-glycan sialylation by at least an order of magnitude, indicating a substantial improvement in both potency and selectivity when compared to the unmodified parent bile acid. Molecular docking analysis supported the stronger binding of the synthetic analogue in the enzyme active site. Treatment with SPP-002 also hampered the migration, adhesion, and invasion of MDA-MB-231 cells in vitro by suppressing the expression of signaling proteins involved in the cancer metastasis-associated integrin/FAK/paxillin pathway. In totality, these findings offer not only a novel structural scaffold but also valuable insights for the future development of more potent and selective ST inhibitors with potential therapeutic effects against tumor cancer metastasis.

关键词： Cancer metastasis Integrin-FAK-paxillin signaling pathway Lithocholic acid Sialyltransferase inhibitor

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Author Correction: Engineered droplet-forming peptide as photocontrollable phase modulator for fused in sarcoma protein

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Nature communications 2024年第1期15卷 7213页

作者： Hao-Yu Chuang Ruei-Yu He Yung-An Huang Wan-Ting Hsu Ya-Jen Cheng Zheng-Rong Guo Niaz Wali Ing-Shouh Hwang Jiun-Jie Shie Joseph Jen-Tse Huang Institute of Chemistry Academia Sinica Taipei 115 Taiwan. Chemical Biology and Molecular Biophysics Taiwan International Graduate Program Academia Sinica Taipei 115 Taiwan. Department of Chemistry National Tsing Hua University Hsinchu 300 Taiwan. Neuroscience Program of Academia Sinica Academia Sinica Taipei 115 Taiwan. Institute of Molecular Biology Academia Sinica Taipei 115 Taiwan. Institute of Physics Academia Sinica Taipei 115 Taiwan. Institute of Chemistry Academia Sinica Taipei 115 Taiwan. jthuang@gate.sinica.edu.tw. Neuroscience Program of Academia Sinica Academia Sinica Taipei 115 Taiwan. jthuang@gate.sinica.edu.tw. Sustainable Chemical Science and Technology Taiwan International Graduate Program Academia Sinica Taipei 115 Taiwan. jthuang@gate.sinica.edu.tw. Department of Applied Chemistry National Chiayi University Chiayi City 600 Taiwan. jthuang@gate.sinica.edu.tw.

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Cover Feature: Donor-Reactivity-Controlled Sialylation Reactions (Eur. J. Org. Chem. 32/2021)

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European Journal of Organic Chemistry 2021年第32期2021卷

作者： Dr. Kesatebrhan Haile Asressu Dr. Chun-Wei Chang Dr. Sarah Lam Prof. Cheng-Chung Wang Institute of Chemistry Academia Sinica Taipei 115 Taiwan Taiwan International Graduate Program (TIGP) Sustainable Chemical Science and Technology (SCST) Academia Sinica Taipei 115 Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu 300 Taiwan

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Rapid and highly efficient adsorption of dye and heavy metal on low-cost adsorbent derived from human feces and Chlorella vulgaris

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Environmental Nanotechnology, Monitoring and Management 2023年 20卷

作者： Wibowo, Yudha Gusti Lululangin, Bonifasius Revo Gifta Safitri, Hana Rohman, Arif Sudibyo Priyanto, Sugeng Syarifuddin, Hutwan Tatik Maryani, Anis Tawfiqurahman Yuliansyah, Ahmad Kurniawan, Ade Tsabitah, Natasya Taher, Tarmizi Petrus, Himawan Tri Bayu Murti Sustainable Mining and Environmental Research Group Department of Mining Engineering Institut Teknologi Sumatera Jl. Terusan Ryacudu Way Huwi Kec. Jati Agung Kabupaten Lampung Selatan Lampung 35365 Indonesia Center for Green and Sustainable Materials Institut Teknologi Sumatera Jl. Terusan Ryacudu Way Huwi Kec. Jati Agung Kabupaten Lampung Selatan Lampung 35365 Indonesia Departement of Chemical Engineering Universitas Gadjah Mada Jl Grafika No. 2 Sleman Bulaksumur 55284 Indonesia Department of Geomatic Engineering Institut Teknologi Sumatera Jl. Terusan Ryacudu Way Huwi Kec. Jati Agung Kabupaten Lampung Selatan Lampung 35365 Indonesia Research Center for Mining Technology - National Research and Innovation Agency Jl. Ir. Sutami KM. 15 Tanjung Bintang South Lampung Lampung 35361 Indonesia Department of Mechanical Engineering Universitas Negeri Jakarta Jakarta Indonesia Postgraduate Program of Environmental Science Universitas Jambi Jambi Indonesia Department of Environmental Engineering Institut Teknologi Sumatera Jl. Terusan Ryacudu Way Huwi Kec. Jati Agung Kabupaten Lampung Selatan Lampung 35365 Indonesia

Wastewater management is a pressing global concern, demanding effective, efficient, cost-friendly, and user-friendly solutions. Among the various methods available, adsorption has emerged as a practical choice. The primary culprits responsible for many human diseases in wastewater are heavy metals and dyes. In this study, we successfully harnessed low-cost biochar derived from human feces and Chlorella vulgaris to significantly accelerate and enhance the removal of heavy metals and dyes. Human feces and Chlorella vulgaris were transformed into biochar under three distinct conditions: biochar, Chlorella vulgaris, and a combination of both. Notably, these materials exhibited exceptional capabilities, removing heavy metals and dyes by as much as 98 % within a mere 10-minute timeframe. This material have adsorption capacity up to 56.8 mg/g for Mn and 20 mg/g for Methylene Blue. To comprehensively evaluate the performance of the optimal samples, we conducted a battery of tests, including performance assessments, sorption capacity measurements, exploration of five isotherm models, and kinetic analyses. Furthermore, we elucidated the sorption mechanisms through thorough characterizations of the materials using SEM, XRD, FTIR, and XRF, providing holistic insights into their properties. This study extends its relevance beyond the laboratory, offering valuable insights into future prospects and policy recommendations. In doing so, it serves as a pivotal resource for researchers and governmental bodies alike, facilitating progress in wastewater treatment and environmental policy development. © 2023 Elsevier B.V.

关键词： Adsorption Biochar Dye sorption Heavy metal sorption Nanocomposite material Wastewater

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