APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Jieying Wan,Hao Zhang,Ji Yang,Jiageng Zheng,Zhongkang Han,Wentao Yuan,Bingru Lan,Xiaodong Li
Electrochemical nitrate to ammonia conversion provides an eco-friendly route for a highly valued product. However, nitrite intermediate formation and hydrogen evolution competition hinder full conversion. Here, we implement a Fe-Mo dual single-atom catalyst where the two metals work in tandem to achieve nitrate to ammonia conversion with excellent activity and stability, an ammonia yield rate of up to 13.56 mg cm −2 h −1 and a Faradaic efficiency up to 94%. In-situ Raman and Fourier-transform infrared spectroscopy confirms nitrite as the intermediate bound to metal sites. Time-dependent detection of products and DFT calculations support a tandem mechanism: the Mo single atoms are the preferred sites for the conversion of nitrate to nitrite, while the Fe single atoms catalyze the further conversion of nitrite to ammonia. This discovery paves the way for energy-relevant transformations using bimetallic single-atom catalysts.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2024
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IF 3.9
Tingting Xiang,Qingchao Zhu,Tanyu Zhou,Chenglong Chen,Ruibo Wang,Tieyu Hu,Bing Li,Ziwei Xu,Juan Yang
Graphical Fe−N−C catalysts, doped with phosphorus, show improved ORR activity. Fe-NPC catalyst exhibits high metal loading, excellent ORR performance (onset potential of 1.00 V, half-wave potential of 0.864 V), and promising application in Zn-air batteries (758.8 mAh g −1 Zn ). DFT calculations reveal that phosphorus enhances O 2 activation and reduces the energy barrier for the rate-determining step. Atomically dispersed iron and nitrogen co-doped carbon materials (Fe−N−C) represent promising non-precious metal catalysts for the oxygen reduction reaction (ORR), offering potential alternatives to noble metal-based benchmarks. In our study, we investigated the influence of phosphorus doping on the catalytic activity of Fe−N−C. The experimental research demonstrate that the doping of phosphorus significantly enhances the ORR activity. Specifically, the resulting Fe-NPC exhibits high metal loading and excellent ORR activity in 0.1 M KOH with an onset potential of 1.00 V and a half-wave potential of 0.864 V. Density functional theory (DFT) simulations reveal that phosphorus improves the electrocatalytic activity by activating O2 molecules and reducing the energy barrier (the hydrogenation reaction *OH→H2O) of the rate-determining step. Furthermore, Fe-NPC exhibits promising application prospects as an air cathode in Zn-air batteries, delivering a high maximum discharge power density of 180.3 mW cm −2 and outstanding discharge specific capacity (758.8 mAh g −1 Zn ) at a discharge current density of 10 mA cm −2 .
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Chem
·
2022
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IF 25.832
Bo Wu,Tiejun Lin,Zhengxing Lu,Xing Yu,Min Huang,Ruoou Yang,Caiqi Wang,Chen Tian,Jiong Li,Yuhan Sun,Liangshu Zhong
Summary The direct conversion of methane to C2 oxygenates with high selectivity under mild conditions has attracted wide attention but still remains a great challenge. Herein, we report the conversion of methane to acetic acid (CH 3 COOH) with ultrahigh selectivity for oxygenated products by the direct coupling of CH 4 , CO, and H 2 O 2 over ZSM-5-supported Fe binuclear sites under 30°C. The unexpected ultrahigh selectivity toward CH 3 COOH was attributed to the unique Fe binuclear site structure of [Fe(III)–( μ O) 2 –Fe(III)–(OH) 2 ], which was evidenced by advanced spectroscopic techniques and density functional theory (DFT) calculations. It was suggested that the lower energy barriers for the direct coupling of methyl radicals (·CH 3 ) and adsorbed CO∗ and OH∗ species to form CH 3 COOH, compared with the oxidation of CH 4 by OH∗ to form CH 3 OH, benefited the CH 3 COOH formation.
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Materials Chemistry Frontiers
·
2024
·Vol. 8
·期 10
·2282-2292
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IF 6
Congcong Lu,Yu Yang,Songjun Li,Maiyong Zhu
Because of their superior power and energy densities, supercapacitors have garnered considerable amounts of attention in energy storage technologies. Co3O4 is considered as a regularly used electrode material for supercapacitors because of its high theoretical capacitance and outstanding electrochemical activity. However, owing to the Co3O4 electrode materials’ rapid capacity decay and low intrinsic conductivity, it is challenging to achieve high theoretical capacitance. As a result, doping Co3O4 with metal components can enhance its electrical and surface characteristics while also raising its conductivity. Through a straightforward hydrothermal reaction and subsequent thermal decomposition, a series of Fe doping into Co3O4 has been successfully realized in this paper. This generates a nanosheet floral cluster structure and exposes more active sites, and the two metal elements work in concert to improve the capacitance performance. The electrochemical performance of the Co-0.2Fe-450 electrode material appears satisfactory when the doping amount of Fe is 0.2 mmol and its thermal decomposition temperature is 450 °C. The specific capacitance at 1 A g−1 is 680 F g−1. The capacitance retention rate at 10 A g−1 current density after 5000 charge–discharge cycles is 84.67%. Notably, the assembled asymmetric supercapacitor retains 105.5% of its capacitance after 5000 cycles and has a power density of 803.13 W kg−1 and an energy density of 17.78 W h kg−1. Fe-doped Co3O4 has a strong future in energy storage, as evidenced by its exceptional electrochemical characteristics.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Huiyu Sun,Xinyu Gu,Jun Yu,Nannan Zhang,Zhengying Wu,Jiawei Qiang,Zhongjie Song,Yukou Du
The oxygen evolution reaction (OER), as the core half-reaction in water electrolysis (WE), plays a decisive role in determining the overall efficiency of hydrogen production. Cobalt carbonate hydroxide (CoCH) has recently emerged as a attractive material for alkaline OER due to its robust structural stability. In this study, urchin-like CoCH was employed as a precursor template to synthesize Fe and Mn co-modified CoCH catalyst on nickel foam (NF) through Mn-doping and surface Fe-modification strategies (recorded as Fe,Mn-CoCH/NF). This optimized hierarchical structure enhanced the exposure of active sites and facilitated faster electron/mass transport paths. The incorporation of Fe and Mn effectively regulated the position of d-band center and facilitated a more efficient lattice oxygen mechanism (LOM) for OER, thereby enhancing the intrinsic activity of the catalyst. Compared to the unmodified CoCH/NF, the Fe,Mn-CoCH/NF exhibited significantly improved OER catalytic activity, characterized by a substantially reduced overpotential (204 mV at 10 mA cm −2 ) in alkaline electrolyte, alongside remarkable stability. Utilizing this catalyst, an overall water splitting (OWS) system was further developed, capable of driving efficient OWS at a low cell voltage (1.49 V at 10 mA cm −2 ). Furthermore, the unique hierarchical structure of Fe,Mn-CoCH/NF contributed to mitigating electrochemical corrosion and the toxic effects of Cl − during seawater electrolysis, enabling the catalyst to maintain excellent catalytic activity and stability even in alkaline seawater system.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2025
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IF 4.6
Xueyi Ren,Honglei Tian,Jianke Li,Yuhuan Zhang
Colorimetric detection methods are prosperous in the monitoring of contaminants in food and environmental matrices. However, the traditional single-channel color changes seriously restrict the enhancement of their sensitivity and facile applications. Herein, a Fe 3+ concentration-controlled dual-channel ratiometric colorimetric sensing platform for the sensitive detection of Pb 2+ was established. Generally, the low concentrations of Fe 3+ can trigger a typical absorption peak at 652 nm of the oxidized TMB (oxTMB). While high concentrations of Fe 3+ induce colorless-to-orange change due to the generation of biphenyl quinone with strong absorption peaks at 450 nm. Interestingly, the presence of Pb 2+ could convert Fe 3+ to Fe (3+x)+ by a displacement reaction, causing a blue-to-colorless change at low Fe 3+ concentrations or an orange-to-blue color change at high Fe 3+ concentrations. The latter dual-channel color variances corresponded to a more distinguished visual quantification of Pb 2+ compared to the former one-channel changes. As such, the Pb 2+ was detected over a range of 0.625-25 µM, with a low detection limit (LOD) of 70 nM. Additionally, by integrating smartphone optical equipment and color recognition software, an intelligent platform for the instant detection of Pb 2+ was established, with a LOD of 0.30 µM. In real samples detection, the developed smartphone sensing platform demonstrated excellent recovery rates (89.0±4.6% to 111.1±7.4%), comparable to the conventional UV-Vis spectroscopy. This work sheds light on fabrication dual-channel colorimetric detection methods for enhanced sensing performance and provides a rapid, sensitive, and intelligent platform for detecting small molecular hazards in the environment.
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ACS Applied Nano Materials
·
2025
·
IF 5.5
Haoming Xie,Lifen Su,Yulong Yang,Jibin Miao,Ru Xia,Jiasheng Qian,Lei Miao
Water scarcity and pollution are the challenges most countries face around the world, especially the large amount of organic wastewater. Solar-driven evaporation is an environmentally friendly and high-performance technology of freshwater production. However, photothermal materials fail when the water includes complex recalcitrant pollutants such as tetracycline hydrochloride (HCL-TC) and bisphenol A (BPA). Here, Fe@carbon nanotube (Fe@CNT) arrays were prepared in situ by using acetonitrile as the carbon source and ferrocene as the catalyst, followed by further solar-driven water evaporation and photo-Fenton catalytic degradation of organic pollutants synergistically. Owing to the Fenton effect and excellent solar absorption, Fe@CNTs accelerate the separation of photogeneration electron–hole pairs to improve the degradation of organic pollution and production of freshwater. Therefore, the Fe@CNT layers show outstanding solar absorption and hydrophilicity, resulting in a high solar evaporation efficiency of 94%. Meanwhile, the degradation efficiencies of organic pollutants (methylene blue, HCL-TC, and BPA) are more than 99% due to the synergistic effect of photothermal and photo-Fenton-catalysis effects. This work provides a promising strategy for the treatment of organic wastewater in an environmentally friendly way.
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Journal of Cleaner Production
·
2023
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IF 11.1
Shu Wang,Nanqi Ren,Danhui Liang,Jifei Chang,Xin Wang,Jiaguo Yan,Xiang Cheng,Lili Dong,Nan Li
Vivianite is an important bio-induced product of dissimilated iron reduction (DIR), which exists widely in activated sludge and digested sludge of wastewater treatment plants (WWTPs). Extracellular polymeric substances (EPS) surrounding dissimilatory iron-reducing bacteria (DIRB) were reported to be transient media for microbial extracellular electron transfer (EET) and DIR. However, what happens when a layer of EPS envelops microbial cells during vivianite recovery? This study tried to assess the relationship between iron reduction and electron transfer by stripping EPS layer-by-layer, then clarified the delamination of different EPS layers on the performance of vivianite recovery. After stripping total EPS (PC-EPS batches) of DIRB, the Fe (III) reduction efficiencies ( R Fe ), Fe (III) reduction rate ( V Fe ), and vivianite formation efficiency ( R V ) decreased by 33%, 37%, and 30%, respectively. Tightly bound-EPS (TB-EPS) was confirmed to play a crucial role in vivianite formation, which contributed 28–51% to vivianite recovery and 34–55% to iron reduction. Electronic shuttle substances were contained in TB-EPS, which enhanced the EET rate and efficiency between cells and Fe (III). The polysaccharide content of TB-EPS was positively related to adhesiveness between cells and mineral, as well as the iron reduction efficiency. Furthermore, redox proteins (PpcA, OmcB) were embedded in EPS, which shortened the distance of electron hopping to across the EPS layer and further accelerated vivianite recovery from wastewater. Long-term operation of anaerobic reactors confirmed that TB-EPS played critical roles in bio-induced vivianite formation.
研究领域:
环境科学
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微生物学
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污水处理
·
生物地球化学
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Zhiheng Pang,Fang Cui,Qinghai Ma,Tieyu Cui
As an alternative to noble metal oxygen evolution reaction (OER) catalysts, iron-based materials face limitations in their practical applications due to their relatively low activity and conductivity, despite their cost-effectiveness. In this study, we developed a Ce-doped amorphous FeOOH catalyst (Ce-FeOOH) using an electron modulation strategy, leveraging the strong electron-absorbing capability of Ce 4+ ions to regulate the electronic structure of the FeOOH active site. Experimental results and characterizations demonstrated that Ce 4+ extract electrons from the iron sites via the Ce(IV)-O-Fe electronic bridges, generating highly active iron species with elevated oxidation states, thereby effectively enhancing the OER catalytic performance. The optimized Ce-FeOOH-3:2 exhibited outstanding OER performance in 1.0 M KOH, achieving a low overpotential of 248 mV at a current density of 10 mA cm −2 , a Tafel slope of 44 mV dec −1 . Moreover, the material exhibits stable continuous electrolysis performance for 100 h at overpotentials of 250 mV and 384 mV, respectively. This work provides a novel approach to synergistically modulating the electronic state of iron-based catalysts through high-valent metal doping and structural amorphization, offering valuable insights of the design and development of highly efficient and stable non-precious metal OER catalysts.
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ACS Sensors
·
2024
·
IF 8.2
Fan Shi,Zejun Zhang,Behisht Ara,Zhitan Huang,Qifeng Gui,Ahmad Mansoor,Wei Sun
Fe single-atom and Fe cluster-coupled N, S co-doped carbon nanomaterials (FeSA–FeONC-NSC) were prepared through a two-step high-temperature pyrolysis process using Gelidium corneum enriched with C, Fe, O, N, and S as precursors. The analysis by aberration-corrected scanning transmission electron microscopy and X-ray absorption spectroscopy revealed the presence of single-atom Fe in Fe–N4 coordination structures, along with small clusters as Fe–O-coordinated Fe2O3. Single-atom Fe in the form of Fe2+/Fe3+ provides more electrocatalytic active sites, which synergistically accelerates the charge migration process in the assembly of FeSA–FeONC-NSC with Fe2O3 clusters. The flexible nonenzymatic sensor, based on FeSA–FeONC-NSC and fabricated using a polydimethylsiloxane substrate, exhibited excellent catalytic activity for both uric acid (UA) and tyrosine (Tyr). Low detection limits for UA (0.14 μmol L–1) and Tyr (0.03 μmol L–1) were observed by using chronoamperometry in artificial sweat. The in situ detection of sweat was performed in combination with an integrated circuit board affixed to human skin, and the results were generally consistent with those of the high-performance liquid chromatography method. Therefore, FeSA–FeONC-NSC serves as a good modifier for wearable electrochemical sweat sensor applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Rong Li,Yiziqi Lu,Meiqian Lu,Yue Liu,Guodong Zhang,Qiuling Ma,Jian Zhou,Tiecheng Wang
Iodinated X-ray contrast media, as a frequently used medical diagnosis in the imaging of internal organs, soft tissues, and blood vessels, are widely encountered in water environments because of their non-metabolic ability. Herein, a series of co-precipitates (DBC-FeO x ) of dissolved black carbon (DBC) and FeO x were successfully synthesized. The chelation of Fe species with COO – groups in DBC enhanced the excellent electron transfer capability and persulfate (PS) activation performance of the resulting DBC-FeO x , thus boosting iopamidol (IPM) degradation. The IPM removal rate constant in the DBC-FeO x /PS was 35 times and 4.6 times higher than those observed in the DBC/PS and FeO x /PS systems, respectively. There existed an appropriate C/Fe molar ratio in the DBC-FeO x co-precipitates for PS activation, and the IPM degradation was driven by both radical and non-radical pathways. Fe sites were the primary active sites in DBC-FeO x for PS activation, and C=O groups played an important role in accelerating the Fe(III)/Fe(II) cycle by promoting rapid electron transfer, thereby enhancing radical oxidation pathways. Concurrently, DBC-FeO x acted as an electron shuttle to promote the electron transfer from IPM to PS, creating non-radical pathways for IPM removal. IPM degradation processes involved amide hydrolysis oxidation, hydrogen extraction, and deiodination. The typical iodine species HOI was also converted to non-toxic IO 3 - after IPM decomposition, thus reducing potential risks.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 14
·21430-21441
·
IF 0
Jiang Changjin,Zhang Shuang,Zhang Ting
Fe 3+ complexed with 3-aminopropyltriethoxysilane (APTES)-modified carboxymethyl chitosan (CMC) named Fe-ACMC was synthesized by a one-step method at room temperature and pressure. The surface morphology and chemical structure of Fe-ACMC were characterized by SEM-EDS, XRD, BET, FT-IR, XPS, and ζ-potential. In batch adsorption, the optimum pH for arsenate [As(V)] adsorption onto Fe-ACMC was 3–9 with removal efficiency > 99%. The adsorption of As(V) could reach equilibrium within 25 min and the maximum adsorption capacity was 84.18 mg g –1 . The pseudo-second-order model fitted well the kinetic data ( R 2 = 0.995), while the Freundlich model well described the adsorption isotherm of As(V) on Fe-ACMC ( R 2 = 0.979). The co-existing anions (NO 3 – , CO 3 2– , and SO 4 2– ) exhibited a slight impact on the As(V) adsorption efficiency, whereas PO 4 3– inhibited As(V) adsorption on Fe-ACMC. The real applicability of Fe-ACMC was achieved to remove ca. 10.0 mg L –1 of As(V) from natural waters to below 0.05 mg L –1 . The regeneration and reuse of Fe-ACMC for As(V) adsorption were achieved by adding 0.2 mol L –1 HCl. The main adsorption mechanism of As(V) on Fe-ACMC was attributed to electrostatic attraction and inner-sphere complexation between –NH 2 ···Fe 3+ and As(V). In fixed-bed column adsorption, the Thomas model was the most suitable model to elucidate the dynamic adsorption behavior of As(V). The loading capacity of the Fe-ACMC packed column for As(V) was 47.04 mg g –1 at pH 7 with an initial concentration of 60 mg L –1 , flow rate of 3 mL min –1 , and bed height of 0.6 cm. Graphical abstract
研究领域:
环境科学
·
材料科学
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