INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Shaowu Yuan,Yihui Wu,Wenjing Chen,Zhanyuan Xu,Yuxin Wang
The development of an efficient yet cost-effective non-precious electrocatalyst for the hydrogen evolution reaction (HER) in alkaline water and seawater systems remains a formidable obstacle to the large-scale production of hydrogen energy, stemming from the sluggish kinetics of electron transfer reactions during the HER process. In this article, an amorphous Co-P-W electrocatalyst on nickel foam is prepared using a brief cyclic voltammetry (CV) electrodeposition method. The optimized Co-P-W electrocatalyst exhibits excellent electrocatalytic performance for HER, which only requires overpotentials of 59 and 143 mV to achieve a current density of 10 mA cm −2 in alkaline water (1.0 M KOH) and alkaline seawater (1.0 M KOH + natural seawater), respectively, and remarkable stability and durability. The improved HER performance of the Co-P-W electrocatalyst is attributed to the introduction of W, which modulates the electronic structure of Co and P, optimizes the adsorption/dissociation of H 2 O, and reduces the charge transfer resistance of the Co-P electrocatalyst, thus improving the kinetics of the HER. Furthermore, the W-doping significantly enhances the hydrophilicity of the Co-P electrocatalyst, which favors rapid and thorough penetration of electrolytes into the electrocatalyst, facilitating the formation of a highly accessible reaction interface, ultimately resulting in excellent HER activity. Our findings demonstrate the feasibility of designing an efficient, durable, and scalable electrocatalyst to significantly boost HER efficiency for practical water electrolysis.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Xiaofang Pan,Hong Ma,Rongning Zhang,Ran Deng,Meng Li,Binfei Yang,Ruiying Zhu,Li Zhao,Yong Liu,Xiaobo Gong
In this study, a manganese co-doped with phosphorus and nitrogen pigeon guano-derived biochar catalyst (Mn/PN-PGC) was constructed for the rapid removal of tetracycline hydrochloride (TC) by activated periodate (PI). The results show that the Mn/PN-PGC materials obtained after Mn doping have increased defects and a higher specific surface area, resulting in more PI catalytic active sites. At room temperature, 0.1 g·L −1 of Mn/PN-PGC and 0.1 g·L −1 of PI could achieve 92.2 % TC removal efficiency with a rate constant of 0.257 min −1 . The removal of TC remained above 84.32 % over a wide pH range. EPR tests, quenching experiments, probe experiments and electrochemical tests demonstrated the mechanism of the synergistic degradation of TC by radical (IO 3 •/•O 2 − /•OH) and non-radical of electron transfer. Additionally, the ecotoxicity was reduced after treatment with the Mn/PN-PGC/PI system, with no toxic reactive iodine production detected. The resourceful utilization of agricultural wastes in this study can alleviate the problem of agricultural waste management, promote sustainable practices, and ultimately facilitate the evolution of advanced and sustainable methods for the remediation of antibiotics in wastewater.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Xiaoyue Chen,Guangmin Ren,Yaru Wang,Zizhen Li,Zisheng Zhang,Xiangchao Meng
The synthesis of ammonia through electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is a presumable strategy. However, it still faces the problems of poor activity and low Faradic efficiency, so the development of efficient, stable and highly selective catalysts is of the importance. Molybdenum disulfide (MoS 2 ) materials are widely used in NRR reactions owing to good electrical conductivity and abundant active sites, but the edge active site is the dual active site of NRR and competitive hydrogen evolution reaction (HER). Encouragingly, the strong interaction between elements in the P-block and N 2p orbitals results in excellent performance in adsorbing and activating nitrogen. Meanwhile, the partial occupation of p-orbitals by elements in the P-block also leads to poor HER activity. Herein, we introduced the P-block element Bi into 1 T-MoS 2 and prepared Bi 2 S 3 /MoS 2 composite. Taking advantage of the high conductivity of 1 T-MoS 2 and the N 2 adsorption and activation advantages of Bi element, an ammonia yield rate of 54.64 µg h −1 mg −1 cat. and a high Faradic efficiency of 58.56 % were obtained. In addition, the active site and the evolution pathway of N 2 reduction were investigated by in-situ infrared spectroscopy measurements and density functional theory (DFT). The in-situ infrared spectroscopy measurement results manifested the presence of the main intermediate transition state during the reduction of N 2 to NH 3 . The calculation results indicated that N 2 had the best adsorption on the introduced P-block element Bi, and the entire NRR reaction process followed an alternating pathway. This study reveals the synergistic effect of P-block elements and transition metal-based electrocatalytic materials on nitrogen reduction to ammonia synthesis .
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
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2024
·Vol. 130
·期 4
·1-10
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IF 2.5
Song Wenqiang,Zhao Fengjiao,Xu Changyuan,Wang Qun,Yin Hongming
For photoluminescence (PL) properties of Mn 2+ in glass–ceramics are highly dependent on the concentration of Mn 2+ , we experimentally observed the change of Mn 2+ structures from isolated Mn 2+ ion as a tetrahedron, octahedron to Mn 2+ -Mn 2+ dimer in B-P-Zn-K based glass–ceramics with characteristic PL peaks locating at 504 nm, 600 nm, and 660 nm, respectively. Spectral results reveal that condensed Mn 2+ would lead to redshift of PL emission and reduced Luminous intensity caused by concentration quenching, however, with increasing Mn 2+ content, shift of Mn 2+ structure is the determining factor for PL redshift. Moreover, compared with tetrahedral and octahedral Mn 2+ , Mn 2+ -Mn 2+ dimer exhibits highly enhanced PL emission and shortened life span which reveal that transitions of Mn 2+ -Mn 2+ dimer are far more efficient than those transitions in tetrahedral and octahedral Mn 2+ . This enables tuning of color and efficiency of PL emission for Mn-doped glass–ceramics via a simple method. Graphical abstract
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ENVIRONMENTAL RESEARCH
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2024
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IF 7.7
Shi-Wen Lv,Jialu Pan,Xiaoran Wang,Yifan Shao,Yanqing Cong,Lin Che
It is of great significance to establish an effective method for removing Cr(VI) from wastewater. Herein, Fe-doped g-C 3 N 4 (namely Fe-g–C 3 N 4 –2) was synthesized and then employed as photocatalyst to conduct the test of Cr(VI) reduction. Notably, the embedding of Fe ion in g-C 3 N 4 can offer the Fe 2+ /Fe 3+ redox couples, so reducing the interfacial resistance of charge transfer and suppressing the recombination of photogenerated electrons and holes. The impurity energy levels will form in g-C 3 N 4 after the introduction of Fe ion , thereby boosting the light absorption capacity of catalyst. Thus, Fe-g–C 3 N 4 –2 showed good performance in photocatalytic Cr(VI) reduction, and the reduction efficiency of Cr(VI) can reach 39.9% within 40 min. Different with many previous studies, current work unexpectedly found that the addition of p -benzoquinone (BQ) can promote the Cr(VI) reduction, and the reduction efficiency of Cr(VI) over Fe-g–C 3 N 4 –2 was as high as 93.2% in the presence of BQ (1.5 mM). Further analyses showed that BQ can be reduced to hydroquinone (HQ) by photogenerated electrons, and UV light can also directly induce BQ to generate HQ by using H 2 O as the hydrogen donor . The HQ with reducing ability can accelerate the Cr(VI) reduction. In short, current work shared some novel insights into photocatalytic Cr(VI) reduction in the presence of BQ. Future research should consider possible reactions between photogenerated electrons and BQ. For the UV-induced photocatalysis , the suitability of BQ as the scavenger of O 2 •‒ must be given carefully consideration.
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高影响因子
APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Huayi Cai,Hui Zhang,Nan Gao,Yi Fang,Xinjian Xie,Yulong Fang,Guifeng Chen
Exploring green methods for removing organic pollutants from water bodies has attracted significant attention. In this research, N-ZnO/p-BN adsorption-photocatalytic composites were prepared by a simple solvothermal method, and various analytical characterizations confirmed the formation of B-O-Zn bonds at the heterojunction interface that facilitated the separation of photogenerated carriers and revealed a type-II mechanism of charge transfer in the heterostructure. The photodegradation efficiency for oxytetracycline (OTC) by composites with different N-ZnO loadings was investigated under simulated sunlight, and the degradation efficiency of the optimal sample (50 wt% N-ZnO/p-BN) for 50 mg/L OTC reached 92.2 % at 120 min. Efficient pollutant enrichment, broadened light absorption range, high dispersion of the photocatalysts, and effective charge migration are all important factors for improving photocatalytic activity. Furthermore, the photocatalytic process was further investigated, experiments showed that the N-ZnO/p-BN composites were universally applicable under a variety of conditions and possessed the characteristics of low dosage and high degradable concentration. Finally, a rational photocatalytic mechanism was proposed for the degradation system and the degradation pathways of the main degradation model OTC were analyzed and deduced. Therefore, this study provides new ideas for designing high-performance adsorption-photocatalytic composites.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Ne Ni,Ying Ouyang,Jianqiang Liu,Enhui Xing,Yibin Luo,Xingtian Shu
It was the thermostability and acidity of P precursors that influenced the interaction between P species and framework Al to determine the hydrothermal stability of P modified ZSM-5. With H3PO2 and NH4H2PO2 as P precursors, the P–Al interactions of P modified ZSM-5 samples calcined under different temperatures were systematically investigated by X-ray fluorescence, X-ray photoelectron spectroscopy, 27Al, and 31P MAS NMR spectroscopy, and temperature-programmed desorption of NH3 (NH3-TPD). With H3PO2 as the precursor, lower calcination temperature favored less self-polymerization of P species; however, obvious loss of phosphorus was observed during hydrothermal treatment. Conversely, higher calcination temperature tended to result in excessive interaction between P and framework Al for dealumination. Therefore, moderate interactions between P and framework Al were obtained over H3PO2 modified ZSM-5 calcined at 350 °C, which contributed to weaken the self-polymerization of P species. Compared with H3PO2, neutral NH4H2PO2 generated a relatively weaker P-zeolite interaction, which was less affected by the calcination temperature.
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Advanced Energy Materials
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2024
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IF 24.4
Rongrong Deng,Qibo Zhang
The development of advanced electrocatalysts with exceptional performance at high current densities is pivotal for reducing electric energy consumption in industrial water splitting for hydrogen production. Herein, a flexible one-step electrodeposition approach is developed to synthesize superhydrophilic 3D flower-like clusters of Cu–Co–P nanosheets grown in situ on nickel foam (NF). Introducing Cu into Co–P causes strong electron interactions, forming an electronic configuration favorable for the adsorption and desorption of intermediates, which significantly improves the intrinsic catalytic activity. The as-deposited Cu–Co–P/NF display notable bifunctional catalytic activity with low overpotentials of 259 and 65 mV for the oxygen and hydrogen evolution reactions, respectively, at 10 mA cm −2 . Superwetting 3D flower-like nanostructures are conducive to the penetration of electrolytes and the rapid release of bubbles, enabling the efficient utilization of active sites and the timely release of bubble stress under high current densities. An assembled Cu–Co–P/NF(+, −) electrolyzer achieves an impressive voltage of 1.85 V at 500 mA cm −2 for water splitting and appreciable stability for over 220 h under simulated industrial conditions. This work offers an attractive strategy for regulating superaerophobic Co–P electrocatalysts for industrial water splitting, which can contribute to practical applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Yujie Liu,Yuting Jiang,Yan Meng,Weini Xiong,Ziling Yuan,Ruihua Liu,Chao Yang
Because the interactions among contaminants may lead to enhanced toxicity, combined pollution caused by the co-presence of multiple contaminants has increasingly gained public concern. p -Nitrophenol (PNP) and 1,2-dichloroethane (1,2-DCA) are frequently co-detected in groundwater. To completely eliminate PNP, 1,2-DCA and intermediates from polluted sites, in this study, a novel degrader KTU-PDG was created by functional assembly of PNP and 1,2-DCA biodegradation pathways in a robust chassis Pseudomonas putida KT2440. Cell growth assay indicated that PNP or 1,2-DCA can be metabolized as a sole carbon source by strain KTU-PDG for cell proliferation. Stable isotope analysis indicated that strain KTU-PDG possesses the capability of co-mineralizing PNP and 1,2-DCA to CO 2 in mineral salt medium. In wastewater bioremediation, the strain KTU-PDG was proven to be capable of co-mineralizing PNP and DCA and maintained high cell viability during bioremediation. Herein, we demonstrate for the first time co-mineralization of PNP and 1,2-DCA by a single strain. Moreover, green fluorescent protein (GFP)-labeling of strain KTU-PDG facilitates estimation of viable cell number and real-time monitoring of cellular activity and transfer by autofluorescence in the environment. These merits of strain KTU-PDG highlight great potential of this degrader for in situ bioremediation of sites co-contaminated with PNP and 1,2-DCA. More importantly, this strategy of multi-pathways assembly in an optimal chassis shows good potential for the clean-up of combined pollution caused by other organic pollutants.
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PubMed
高影响因子
Applied Materials Today
·
2024
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IF 7.2
Guobo Huang,Siqi Huo,Jiahao Ren,Wei Chen,Haiqin Yang,Shenwei Xiao,Tianle Wang,Hong Peng,Pingan Song
The nanomaterials have been deeply explored as flame retardants for various polymeric materials due to their multifunctionality, but they often fail to significantly increase the limiting oxygen index (LOI) and vertical burning UL-94 rating, thus unable to meet industrial needs (LOI>27.0 % and UL-94 V-0 rating). Herein, we fabricated a cerium/phosphorus-doped g-C 3 N 4 (Ce/P-CN) nanohybrid as a multifunctional high-efficiency fire retardant for acrylonitrile–butadiene–styrene (ABS). The Ce/P-CN nanoflakes featured a strengthening effect towards ABS, 10 wt% of which increased the tensile strength of ABS/(Ce/P-CN) by 33.8 %. Meanwhile, the ABS/(Ce/P-CN) nanocomposites showed remarkably enhanced high-temperature stability and carbonization performances relative to virgin ABS. Ce/P-CN simultaneously improved the anti-ignition, fire retardancy and smoke suppression of ABS due to the barrier effect of g-C 3 N 4 nanoflakes and the catalytic carbonization effect of cerium and phosphorus. Notably, adding 10 wt% Ce/P-CN increased the LOI and UL-94 rating of ABS to 28.6 % and V-0, respectively, demonstrating its high flame-retardant efficiency. Thus, the high flame-retardant efficiency and multifunctionality enable Ce/P-CN to outperform previous flame retardants for ABS. This work offers a novel strategy for the development of high-efficiency g-C 3 N 4 nanoflakes, which endow ABS with improved mechanical robustness and fire retardancy and show broad industrial prospects.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shi-Ting Huang,Yong-Qian Lei,Peng-Ran Guo,Hong-Xin Chen,Shu-Chai Gan,Zeng-Hui Diao
In this study, a biomass-derived carbon block with heteroatoms (P and S) self-doped graphene structure was successfully synthesized by spent coffee grounds (SCG) directly sintered method. The spent coffee grounds biomass-derived carbon (SCC) block was used as electrocatalytic electrode to effectively degrade the antiviral drug of Favipiravir (FAV) in water, which represented excellent oxygen reduction reaction (ORR) activity with the H2O2 production. The doped heteroatoms in the graphene structure of SCC provided many active sites in the electrocatalytic electrode for ORR as well as more production of reactive OH･. Based on the structural characterization, radical species identification and intermediate products analysis, the reaction mechanism of FAV degradation by the SCC block electrode was proposed. This catalytic system also showed high ecological safety that the ecological toxicity for Vibrio fischeri was significantly reduced with the degradation process of FAV. The degradation of FAV in recycle test and in real sample of lake water, well water, tap water all demonstrated high stability of structure and catalytic activity of SCC. The electrocatalytic system based on SCC block electrode has realized the recycling and utilization of biomass resources and has promising application on the removal of environmental pollutants.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jinmeng Wu,Yujiao Wen,Zihao Leng,Shun Zhang,Shikai Li,Zhonghua Zhou,Zhi Zhou,Nan Zhou
Atrazine (ATZ), a commonly used herbicide, poses significant environmental and health risks due to its persistence in aquatic environments. This study applied peroxymonosulfate-based advanced oxidation technology using N, P-doped rice straw biochar (NP@RSBC700), prepared via one-step pyrolysis, to degrade ATZ. The biochar produced at 700 °C exhibited optimal performance due to its enhanced graphitic structure (I D /I G = 0.77) and physicochemical properties. The NP@RSBC700-activated PMS system achieved a 100 % degradation efficiency of ATZ within a short period of just 2 h. N and P doping synergistically improved active sites, including C O, P-O, graphitic N, pyridinic N, and pyrrole N, alongside a porous structure (180.75 m 2 ⋅g −1 ) and defects, demonstrating the potential of this approach in environmental remediation applications. Liquid chromatography-mass spectrometry revealed three potential ATZ degradation pathways, with reduced intermediate toxicity and bioaccumulation confirming effective detoxification. Hydroponic experiments demonstrated that the biochar not only degraded ATZ efficiently but also mitigated its toxicity on plant seedlings. These findings highlight the multifunctional potential of N, P-doped biochar in PMS-based advanced oxidation processes, combining pollutant degradation with plant health protection.
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