INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Zejie Zhang,Yihui Wu,Deping Zhang
The hydrogen evolution reaction (HER) using earth-abundant noble-metal-free catalysts has gained substantial interest in electrocatalytic water splitting technologies, particularly in water-alkali electrolyzers. The development of highly-efficiency and durable inexpensive electrocatalysts to accelerate the kinetics of HER is still a formidable challenge. In this study, nickel–iron (Ni–Fe) electrocatalyst directly grown on backbones of Ni foam (NF) substrate was facile prepared via one-step potentiostatic electrodeposition method. The obtained Ni–Fe electrocatalyst exhibits a film-like structure. Owing to high electrical conductivity and composition optimization, the synthesized Ni–Fe electrocatalyst with Ni/Fe atomic ratio of c.a. 65:35 possesses an attractive electrocatalytic activity with low overpotentials of 142, 205, and 239 mV at 10, 50, and 100 mA·cm −2 in alkaline electrolyte , respectively.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Liying Wu,Zhiqiang Sun,Yufei Zhen,Shishu Zhu,Chen Yang,Jing Lu,Yu Tian,Dan Zhong,Jun Ma
Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O2 is thermodynamically enabled to capture electrons from Vo to form O2•– under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1O2. In this case, 1O2 and O2•– act as the indispensable intermediate species to accelerate the circulation of O2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nano-confinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.
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高影响因子
Advanced Science
·
2021
·Vol. 9
·期 4
·2104237
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IF 16.806
Qinglin Han,Ximeng Zhao,Yuhong Luo,Lanlan Wu,Shujuan Sun,Jingde Li,Yanji Wang,Guihua Liu,Zhongwei Chen
Rational design of metal oxide supported non-precious metals is essential for the development of stable and high-efficiency oxygen reduction reaction (ORR) electrocatalysts. Here, an efficient ORR catalyst consisting of binary Fe/Co nanoclusters supported by defective tungsten oxide and embedded N-doped carbon layer (NC) with a 3D ordered macroporous architecture (3DOM Fe/Co@NC-WO 2− x ) is developed. The oxygen deficient 3DOM WO 2− x not only serves as a porous and stable support, but also enhances the conductivity and ensures good dispersion of the binary Fe/Co nanocluster, benefiting its ORR catalytic activity. Theoretical calculation shows that there exists a synergistic effect of electron transfer from Fe to Co in the supported binary Fe/Co cluster, promoting the ORR reaction energetics. Accordingly, the 3DOM Fe/Co@NC-WO 2− x catalyst exhibits excellent ORR activity in alkaline medium with a half wave potential ( E 1/2 ) of 0.87 V higher than that of Pt/C (0.85 V). The zinc–air batteries assembled by 3DOM Fe/Co@NC-WO 2− x cathode deliver a higher power density and specific capacity than that of Pt/C. A new strategy of combining synergistic binary-metal nanoclusters and conductive metal oxide support design is provided here to develop efficient and durable ORR electrocatalyst.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Jianan Wang,Jianwei Liu,Qianyue Ma,Xin Chen,Shiyi Sun,Hao Xu,Lei Zhu,Ze Wang,Jiangtao Feng,Wei Yan
Development of high-loading and high-energy-density lithium-sulfur (Li-S) batteries has aroused increasing research interests recently. However, the performance of a conventional two-dimensional Al foil current collector is limited by its smooth/nonporous surface and poor flexibility, which is unfavorable for the achievement of high sulfur loading and sufficient polysulfide adsorption. Hence, a three-dimensional porous Fe-doped polypyrrole aerogel (FPA) is developed by a simple and scalable strategy combing the solution reaction with the freeze-drying technique, aiming at acting as the current collector of cathode to address these issues in Li-S batteries. This FPA possesses a conductive porous network structure with high elasticity and abundant Fe dopants , which can not only buffer the large volume change of sulfur and ensure fast ion/electron transfer, but also effectively anchor the polysulfides and lower the negative polarization effect during cycling. As a result, the FPA@S cathode delivers a high initial capacity of 1196.7 mAh g −1 at 0.2 C and a retained capacity of 829.5 mAh g −1 after 200 cycles, with stabilized Coulombic efficiency and excellent rate performance. This FPA@S cathode also achieves a high cell-level gravimetric energy density of 199.7 Wh kg cell −1 even under a high sulfur-loading (8.57 mg cm −2 ) and low electrolyte/sulfur ratio (6 mL g −1 ), demonstrating its practical potential in future advanced high-energy battery systems.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Pengyu Zhang,Xianfa Zhang,Xiaodan Zhao,Guohua Jing,Zuoming Zhou
Peracetic acid (PAA) is an excellent oxidant that can produce multiple carbon-centered radicals (R•C). A novel advanced oxidation process (AOP) that combines PAA and nanoscale zero-valent iron (i.e. nZVI/PAA) is constructed to evaluate its performance toward tetracycline (TC) abatement. The nZVI/PAA process shows excellent abatement efficacy for TC in the pH range of 3.5–7.5. The presence of humic acid , HPO 4 2− and HCO 3 − exerts inhibitory effects on TC abatement, while the presence of Cl − displays negligible influence in the nZVI/PAA process. Nanoscale zero-valent iron (nZVI) exhibits excellent reusability with no apparent variation in crystallinity . CH 3 C(O)OO• is the predominant active radical that contributes to TC abatement, in which leakage of Fe(II) from the nZVI surface is crucial for a radical generation. Due to the strong complexation tendency of TC towards Fe(II), the Fe(II)-TC complexes are formed, which significantly accelerates the PAA decomposition and TC abatement compared to free Fe(II). In addition, the degradation intermediates of TC are identified, and a possible degradation pathway is proposed. These results will be useful for the application of PAA-based AOPs in the treatment of water containing organic micropollutants.
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Nanomaterials
·
2023
·Vol. 13
·期 13
·1897
·
IF 5.3
Bairui Qi,Qiang Xu,Yunxuan Cao,Zhu Xiao
Copper and iron are the basic metal elements that have attracted much attention in industry. Prussian blue (PB) is a significant class of metal–organic frameworks (MOFs); however, the lack of such linkages between the structure and properties, as well as properties differences, limits their potential applications. In this paper, the Cu-based Prussian blue nanocubes with and without Fe doping were synthesized. With the increasing reaction time, the morphology of the Cu-based Prussian blue nanocubes without Fe doping (PB:Cu NCs) changes from cuboidal to circular, and finally grows back to cuboidal. However, Cu-based Prussian blue nanocubes with Fe doping (PB: CuFe NCs) grow directly from the cube and eventually collapse. The nanocubes show a notable red shift with the tunable spectra from 400 nm to 700 nm. Compared with PB: Cu NCs, the PB: CuFe NCs have higher temperature rise under 808 nm irradiation and better photothermal efficacy. The catalytic efficiency of PB: CuFe NCs changes with the pH and reaches its maximum value of 1.021 mM with a pH of 5.5. The enhanced catalytic reaction by the near-infrared radiation plasmonic photothermal effect is also confirmed. This work highlights the potential of the developed PB: Cu and PB: CuFe NCs for photothermal-enhanced co-catalysis nanomaterials.Keywords:Prussian blue;photothermal effects;catalytic reaction;synergistic action;copper
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Green Energy & Environment
·
2026
·
IF 16.7
Shiteng Tan,Ruikun Wang,Jialiang Dong,Weijie Yang,Zhenghui Zhao,Qianqian Yin,Jun Cheng,Chenliang Ye,Miaolun Jiao
Upgrading sludge to Fe-N-C catalysts via a precoordination-mediated active center evolution strategy • The catalysts possess active sites featuring subnanometer cluster coupled with single atom • DFT reveals electronic coupling effect that enhances ORR kinetic • The catalyst shows superior ORR activity and power output in ZAB and MFC The sluggish kinetics of the oxygen reduction reaction (ORR) remains a critical limitation for green energy conversion technologies. Although Fe-N-C single-atom catalysts offer high atomic utilization, their symmetric coordination environments limit electronic flexibility and catalytic activity. Herein, a precoordination-mediated active center evolution strategy is developed to construct dual scale cluster-single atom Fe-N x active centers using municipal sludge as a low-cost precursor. During the citric acid-assisted hydrothermal process, protein hydrolysis induces the release and redistribution of nitrogen-containing species, forming a precoordinated environment that enables the formation of subnanometer clusters and isolated single-atom sites. Subsequent activation removes mineral species and constructs a hierarchical porous carbon framework with high specific surface area and enhanced mass transport. Density functional theory calculations reveal that electronic coupling between clusters and single atoms induces long-range electronic modulation, shifting the d-band center and optimizing the adsorption energetics of oxygen intermediates. As a result, the catalyst exhibits excellent ORR activity across a wide pH range, delivering a half-wave potential of 0.86 V in alkaline media and outperforming Pt/C in acidic and neutral electrolytes. A Zn-air battery achieves a peak power density of 195 mW cm -2 , while microbial fuel cells deliver 1589 mW m -2 with 54% pollutant degradation. Life-cycle assessment indicates reduced carbon emissions compared with sludge incineration. This work provides a controllable strategy for constructing dual-scale active centers and highlights their promise in green energy conversion and nano-enabled electrocatalysis. Municipal sludge-derived Fe-N 4 single atoms coupled with subnanometer Fe clusters enable electronic coupling, d-band regulation and weakened OH* adsorption, delivering efficient oxygen reduction for zinc-air batteries and microbial fuel cells. Download: Download high-res image (204KB) Download: Download full-size image
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Liyong Du,Yi Liu,Xiufen You,Heming Sun
Metal oxide-based gas sensors are widely used in the detection of toxic and harmful gases due to their advantages of high precision, convenient use and stable performance, but their application range is limited due to the high working temperature. In this work, MOF-derived flower-like Fe-doped Co 3 O 4 porous hollow structures are obtained using a simple solvothermal method . The obtained samples are characterized in terms of their crystalline structure, morphology, chemical composition , optical properties and specific surface area . This study systematically investigates the sensing performance of pristine and Fe-doped Co 3 O 4 samples. The results show that the 2 at% Fe-Co 3 O 4 sample has the best n-butanol sensing properties. This sample exhibits high response and rapid response/recovery speed at a low working temperature of 110 °C, as well as good repeatability and anti-humidity features. The enhanced sensing properties can be attributed to several factors, including the adjustment of baseline resistance, increase in oxygen vacancies , decrease in bandgap, and the formation of unique hollow and porous structures . Overall, this work provides valuable insights into the potential applications of Fe-doped Co 3 O 4 materials in sensing technologies.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 6
·125110
·
IF 7.5
Bingdang Wu,Zihao Cang,Yonghai Gan,Jun Luo,Zhe Li,Zheng Wang,Hongcen Zheng,Minghui Cai,Xiao Luo,Chengcheng Ding,Yibin Cui
Synthesis pathway governs Si-O-Fe bonding uniformity and functional group exposure. • GPFC-H unlocks pH-switchable synergy: charge neutralization (acidic) and hydrophobic association (alkaline). • GPFC-H achieves 91.2% HA removal at pH 6.0 and 74% at pH 9.6, versus < 41% for PFC. • The GPFC-H route requires no post-treatment and is compatible with spray drying. • Spray-dried powder retains > 90% coagulation activity after 28-day storage. Long-chain silane coupling agents like dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride (TPODAC) promise enhanced coagulation performance through hydrophobic interactions, yet their practical application is crippled by uncontrolled hydrolysis and detrimental self-condensation during conventional synthesis. This study demonstrates that the synthesis pathway fundamentally governs Si-O-Fe bonding configuration, colloidal stability, and the resulting coagulation mechanisms. By systematically comparing four synthesis strategies with modulated silane hydrolysis states and component addition sequences, a clear structure-property hierarchy is established through multi-method characterization (FTIR, XPS, XRD, zeta potential) and coagulation performance evaluation. The optimal route, pre-hydrolyzed silane grafted onto pre-formed polymeric ferric chloride (GPFC-H), suppresses silane self-condensation and yields uniform Si-O-Fe covalent bonding with fully exposed quaternary ammonium and C18 hydrophobic chains. This structural perfection unlocks a rare pH-switchable multi-mechanism synergy. At pH 6.0, GPFC-H achieves 91.2% humic acid removal via charge neutralization. Remarkably, at pH 9.6 where conventional coagulants fail (<41% removal), GPFC-H maintains 74% removal through hydrophobic association mediated by its pH-insensitive C18 chains. GPFC-H also achieves 78% Sb(V) removal at pH 7.0, versus 65% for PFC. Furthermore, this synthesis route requires no post-treatment and is compatible with spray drying; the obtained solid powder retains > 90% of its initial activity after 28-day storage, demonstrating its practical potential for industrial production and long-distance transport. By establishing causal links from synthesis pathway to bonding structure to pH-adaptive performance, this work transforms hybrid coagulant preparation from empirical optimization into a designable strategy for advanced water purification. Download: Download high-res image (173KB) Download: Download full-size image
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Zhenhua Hou,Libo Wang,Gang Liu,Ya Wang,Yuhan Wang,Yangyang Zhang,Xiayu Wu,Nan Li
Ammonia has important application value in agriculture and industry as a raw material for producing nitrogen fertilizers and organic chemicals. The Haber-Bosch method is generally utilized to synthesize ammonia through N 2 and H 2 as raw materials in industry, but the process generates serious energy consumption and pollution. In the paper, a heterojunction catalyst is constructed that adopts NH 2 -MIL-125 and Fe-doped W 18 O 49 (Fe-W 18 O 49 ) for photocatalytic nitrogen fixation. Fe-W 18 O 49 is a nanowire containing oxygen vacancies (OVs). OVs can provide active sites for the adsorption and activation of nitrogen gas. The 3D plate-like morphology of NH 2 -MIL-125 can observably reduce the occurrence of nanowires aggregation. This phenomenon can be attributed to NH 2 -MIL-125 playing a supporting role in the fixation of nanowires. New mesoporous are formed between NH 2 -MIL-125 and Fe-W 18 O 49 in the constructed compound catalyst, which can realize efficient mass transfer between the inside and outside of the catalyst. EPR characterization discovers that Fe-W 18 O 49 /NH 2 -MIL-125 cannot produce •O 2 ˗ and •OH radicals. The type II heterojunction forms between Fe-W 18 O 49 and NH 2 -MIL-125. The heterojunction improves the carrier migration path, and the photocurrent intensity is significantly increased. Under simulated sunlight, Fe-W 18 O 49 /NH 2 -MIL-125–2 emerges the best catalytic performance with an ammonia formation rate of 128.2 µmol g −1 h −1 . The yield of ammonia is boosted in comparing with NH 2 -MIL-125 (13 times) and Fe-W 18 O 49 (1.7 times). After several cycles, Fe-W 18 O 49 /NH 2 -MIL-125 remain maintains good stability during the catalytic process. This paper provides a possibility for constructing low-cost heterojunction catalysts in the territory of photocatalytic nitrogen fixation.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xueyan Xue,Nan Xue,Dandan Ouyang,Liuqian Yang,Yanan Wang,Hui Zhu,Aikelaimu Aihemaiti,Jiao Yin
Iron single-atom catalysts (Fe SACs) hold great promise for peroxymonosulfate (PMS) activation and degradation of organic pollutants in wastewater. However, insights into crucial catalytic sites and activation mechanisms of biochar-based Fe SACs for PMS remain a challenge. Herein, cotton stalk-derived biochar-based Fe SACs (Fe SACs-BC) with an asymmetric Fe-N/O-C configuration were prepared, and their PMS activation and acid orange 7 (AO7) degradation mechanisms were investigated. The results showed that the removal efficiency of the Fe SACs-BC catalyst with Fe-N3O-C configuration for AO7 and other five investigated organic dyes reached 95–99% within 15 min. The EPR spectrums, quenching experiments, electrochemical analysis, masking experiments, XPS, and theoretical calculations indicated that degradations of organic dyes were dominated by singlet oxygen, which was generated by direct PMS conversion at the electron-deficient carbon and iron sites in the Fe-N3O-C configuration. The Fe SACs-BC/PMS exhibited high removal efficiency and strong tolerance in different water matrices with a wide pH range, various coexisting anions and interfering substances, showing great potential and applicability for efficient treatment of actual textile wastewaters.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Junjie Qiao,Yuyang Han,Lanyang Feng,Yanting Li,Jianning Ding,Fei Xu,Bencai Lin
This paper reports the low-cost fabrication of high-performance double transition metals (Fe, Ni) and N-doped carbon nanotubes (FexNiy-N-CNT) to catalyze the oxygen reduction reaction (ORR) in zinc–air batteries (ZABs). The target active sites and appropriate carbon substrates of the designed catalysts facilitated charge transfer kinetics. The carbon nanotube (CNT)-based catalysts underwent electrochemical testing using the rotating ring–disk electrode method, and the results revealed that the Fe2Ni1-N-CNT catalyst exhibited both an exceptional ORR performance (E1/2 = 0.86 V) and excellent stability. Furthermore, the ZABs with the Fe2Ni1-N-CNT catalyst exhibited a high power density (169.5 mW cm–2) and an open-circuit voltage (1.46 V). These findings can provide insights into the development of efficient and sustainable CNT-based cathode catalysts for ZABs.
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