ELECTROCHIMICA ACTA
·
2016
·
IF 4.803
Li Shao,Xing Qian,Xiaoying Wang,Hongmei Li,Rucai Yan,Linxi Hou
Highly efficient and low-cost electrocatalysts are essential for producing hydrogen through water electrolysis. Here ternary compounds CoMoS 4 and NiMoS 4 were synthesized by a one-step reaction, and further CoMoS 4 -H and NiMoS 4 -H were obtained by heating the above two samples under Ar atmosphere. The above four materials both show uniformly small irregular nanoparticles. Each element of the four materials exhibits semblable valence without distinct difference of which S was −2, Mo was +6, Ni and Co were +2. We firstly use the above ternary materials as advanced electrocatalysts for HER over a wide pH range, of which CoMoS 4 -H displays the best performance with a low onset overpotential at 8 mV in 1.0 M KOH and 83 mV in 0.5 M H 2 SO 4 . NiMoS 4 -H also shows excellent performance with a low onset overpotential at 26 mV in 1.0 M KOH and 160 mV in 0.5 M H 2 SO 4 . In 1 M phosphate buffer solution, CoMoS 4 -H and NiMoS 4 -H exhibit onset overpotential at overpotential of 122 mV and 152 mV, respectively. These results indicate that the combination of earth-abundant sulfur, cobalt (or nickel) and molybdenum elements can provide highly active electrocatalysts for HER over a wide pH range.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Jiaojie He,Qingwang Cai,Ziyi Kang,Jingxin Zhang,Huan Tang,Tinglin Huang
Research on inorganic metal coagulants has largely focused on the Al, Fe, Ti and Zr-based salts, leaving insufficient studies on the metal Ce. This study first attempted to conduct an in-depth investigation into the coagulation effect of Ce-based reagents with different valence states. The CCl was a pure Ce(III)-based salt, while Ce(IV)/Ce(III) in CAN equaled 2.7/1. The results demonstrated that CAN possessed far superior capability of turbidity removal compared with CCl, which was on par with polyaluminum chloride (PAC). And its ability to remove organic matter even surpassed that of PAC. Furthermore, CAN exhibited more remarkable and stable performance across a broad pH range. Mechanism studies confirmed that the Ce(III) had the strongest organic ligand complexing ability but insufficient hydrolysis ability, leading the complex re-stabilized in solution. Whereas, the merits of Ce(IV) was based on the following distinctive properties: (1) the high positive charge, with zeta potential even close to that of PAC under acidic condition, (2) the readily formed hydrolysis products owning film-like structure to enhance sweep flocculation, (3) the high coordination number to offer abundant reaction sites to balance the three effects, electric neutralization, complexation, and sweeping, to fully exploit their respective advantages. Thus, the above three effects were combined to achieve the stable coagulation efficiency in CAN containing both Ce(IV) and Ce(III), which might be insufficient or competitive in PAC or CCl. The clarification of the coagulation mechanisms is conducive to better developing Ce-based coagulants and may offer valuable insights into finding more suitable metal-based reagents.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Yue Gao,Fang Yang,Hongxian Jian,Kai Zhen,Peng Zhang,Xuejiao Tang,Zhen Fu,Wei Xu,Cuiping Wang,Hongwen Sun
To explore an effective liquid material for the degradation of polycyclic aromatic hydrocarbons (PAHs), sodium citrate (SC) was selected from four kinds of chelating agents for persulfate (PS) activation by transition metals to degrade pyrene in an aqueous system. PS activated by SC chelated ferrous ion (PS/Fe 2+ /SC) can catalyze pyrene degradation under neutral pH, and when the molar ratio of PS, SC, Fe 2+ and pyrene was 2000/2000/2000/1, the maximum degradation percentage reached 94.4% in 720 min through enhancing the PS consumption and oxidative capacity of the system. Furthermore, the pyrene degradation catalyzed by PS/Fe 2+ /SC was not influenced by pH in the range from 3.0 to 11.0, PS/Fe 2+ /SC system could effectively catalyze the pyrene degradation over a wide pH range. Additionally, the presence of 0.1 M of SO 4 2- and H 2 PO 4 - decreased the pyrene degradation using the PS/Fe 2+ /SC system, while 0.1 M of Cl - and NO 3 - had little effect on the pyrene degradation when PS/Fe 2+ /SC was used under neutral pH. Furthermore, pyrene degradation was attributed to the sulfate and hydroxyl radicals produced from PS/Fe 2+ /SC system, and these radicals were detected with strong signals of DMPO-SO 4 and DMPO-OH through electron paramagnetic resonance (EPR) spectroscopy. Finally, seven pyrene degradation products were identified by gas chromatography-mass spectrometer (GC-MS), and a possible pathway of pyrene degradation was proposed.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED GEOCHEMISTRY
·
2024
·
IF 3.1
Yanting Pan,Feng Zhang,Ziyang Zhou,Feng Jiang,Xiaoming Wang,Hui Yin,Wenfeng Tan,Xionghan Feng
A series of cobalt-doped FeS (x% Co–FeS) nanoparticles , prepared via a hydrothermal method, were introduced as catalysts for generating radicals from peroxymonosulfate (PMS) to degrade the endocrine disrupter bisphenol S (BPS) in wastewater. The kinetic results revealed that only a small amount of Co doping (7% At.) could greatly improve the efficiency of PMS activation by FeS, leading to the rapid degradation of BPS (0.21min −1 vs. 0.0046 min −1 ), and no secondary pollution caused by Co leaching. Notably, exceptional activation was observed over a wide pH range from 4 to 11. Moreover, various background ions (NO 3 − , Cl − , CO 3 2− ) and temperatures (10.0–55.0 °C) minimally affected BPS degradation, suggesting excellent applicability in different sewage environments. Furthermore, quenching experiments, coupled with electron paramagnetic resonance technology, identified singlet oxygen ( 1 O 2 ) and sulfate radicals (SO 4 •- ) as the primary reactive oxygen species responsible for BPS degradation. Due to the selectivity of 1 O 2 and the high redox potential of SO 4 •- , this technology had excellent anti-interference and degradation ability. In six repeated batch experiments, the catalysts showed favorable cyclability and stability due to Co(II)/Co(III) cycling mediated by structural S 2− . These results provided insights into the potential applications of modifying natural FeS-type minerals as a promising heterogeneous catalyst for environmental restoration.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2024
·
IF 5.8
Maoyuan Li,Zhongrui Yu,Zulin Sun,Yuchen Liu,Simiao Sha,Jiancheng Li,Riyue Ge,Liming Dai,Bin Liu,Qingqiao Fu,Wenxian Li
Electrocatalyst materials play a crucial role in determining the efficiency of the hydrogen evolution reaction (HER), directly influencing the overall effectiveness of energy conversion technologies. Ni3S2/MoS2 heterostructures hold substantial promise as bifunctional catalysts, owing to their synergistic electronic characteristics and plentiful active sites. However, their catalytic efficacy is impeded by the relatively elevated chemisorption energy of hydrogen-containing intermediates, which constrains their functionality in different pH environments. In order to mitigate this limitation, trace amounts of Pt are introduced into the heterostructure, intending to enhance electronic transport and refining chemisorption energies, thereby facilitating significant enhancements in both HER and oxygen evolution reaction (OER) activities over a wide pH range. It is revealed that the Pt-modified catalyst achieves exceptional HER performance, requiring merely 64 mV and 83 mV overpotentials to attain a current density of 100 mA cm−2 in acidic and alkaline media, respectively. Furthermore, theoretical simulations corroborate that Pt modification optimizes local electronic configurations and augments electronic transfer, contributing to its superior catalytic performance. This investigation underscores the pivotal role of Pt modification in propelling the practical application of Ni3S2/MoS2 heterostructures as highly efficient and pH-universal bifunctional catalysts.
研究领域:
材料科学
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电化学
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能源转换技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 71
·40804-40812
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IF 2.936
Junhui Liu,Long Kong,Xueqiong Huang,Min Liu,Liang Li
In this study, magnetic sulfur-doped Fe3O4 nanoparticles (Fe3O4:S NPs) were applied as adsorbents for the removal of As(V). Fe3O4:S NPs were fabricated by a two-step route, which included low-temperature mixing and high-temperature sintering. The as-prepared Fe3O4:S NPs could effectively remove As(V) under a wide pH range of 2–10 and presented a high As(V) adsorption capacity of 58.38 mg g−1, which was much better than undoped Fe3O4 nanoparticles (20.24 mg g−1). Adsorption experiments exhibited a pseudo-second-order model of adsorption kinetics and a Langmuir isotherm model of adsorption isotherms. Additionally, the coexisting ions such as NO3−, SO42−, and CO32− had no significant effect on As(V) adsorption and the adsorbent worked well in actual smelting wastewater. XPS and FTIR spectra of Fe3O4:S NPs before and after As(V) adsorption showed that Fe–OH groups played a significant role in the adsorption mechanisms. Moreover, the magnetic Fe3O4:S NPs adsorbents after adsorption could be rapidly separated from wastewater with an external magnetic field. Therefore, Fe3O4:S NPs could be an ideal candidate for the removal of As(V) from water.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysts
·
2023
·Vol. 13
·期 3
·552
·
IF 3.9
Bingxin Guo,Chengfei Zhao,Yingshuang Zhou,Junjie Guo,Zhongzhe Wei,Jing Wang
Alkali metals, as ideal electron donors, can effectively regulate the valence state distribution of the host metals. Nevertheless, no studies have reported the application of alkali metal promoters in the hydrogen evolution reaction (HER). Here, we designed an efficient and wide pH-universal hydrogen evolution catalyst that utilizes alkali metal to control the valence, size, and dispersion of Ru NPs. The experimental results reveal that the alkali metal additives contribute to the dispersion and stabilization of metallic Ru. More importantly, the interaction between Na and Ru regulates the distribution of Ru valence states and helps to form more active components of Ru0. Additionally, NaCl functioned as an in situ template to assist the construction of a porous carbon skeleton promotes mass transfer and exposes more active sites, further promoting the synergistic effect of Ru and Na. As a result, the optimal Ru0.3/C−800 delivers high efficiency for HER with an overpotential as low as 29 mV in 1.0 M KOH and 83 mV in 0.5 M H2SO4under 10 mA cm−2. Particularly, the catalytic performance of Ru0.3/C−800 even outbalanced that of commercial Pt/C in an alkaline medium. This rational construction strategy opens up new avenues for obtaining superior pH-universal electrocatalysts.Keywords:alkali metal;Ru based;hydrogen evolution reaction;wide-range pH;promotional effect
研究领域:
化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Progress & Sustainable Energy
·
2013
·Vol. 33
·期 3
·814-823
·
IF 0.865
Ruihua Huang,Bingchao Yang,Qian Liu,Yanping Liu
The simultaneous adsorption of phenol and Cr(VI) from aqueous solution onto this activated carbon/chitosan composite was investigated. This composite almost removes phenol and Cr(VI) simultaneously in a pH range of 2–5. The removals of phenol and Cr(VI) reached up to 95% when phenol and Cr(VI) concentrations were less than 50 mg/L and 200 mg/L, respectively. The presence of phenol reduced Cr(VI) adsorption, while the presence of Cr(VI) had no evident effect on phenol adsorption. The adsorption for both Cr(VI) and phenol followed pseudo-second-order kinetics in single or mixedsystems. © 2013 American Institute of Chemical Engineers Environ Prog, 33: 814–823, 2014
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Qianqian Ni,Xin Ke,Wenjing Qian,Zheng Yan,Jingde Luan,Wengang Liu
A single hydrothermal reaction was used to create BiOI/BiOBr composites, which demonstrated good sunlight-driven photocatalytic degradation activity of tetracycline (TC) over a broad pH range and the degradation efficiency can be stable at about 90%. Moreover,·O 2 - has been identified as the most important active ingredient in the photocatalytic system. Density functional theory (DFT) calculations were used to investigate the electron transfer mechanism of BiOX heterojunctions on a molecular scale, as well as to propose possible photocatalytic degradation mechanisms and reaction sites for tetracycline in different deprotonated forms at a wide range of pH values. The quantitative structure-activity relationship (QSAR) was also used to assess the toxicity of the intermediates. In summary, this study presents new concepts for investigating the photodegradation behavior of antibiotics throughout a wide pH range, which is predicted to be employed for surface water remediation.
研究领域:
环境科学
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材料科学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2015
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IF 6.723
Liang-Liang Feng,Guo-Dong Li,Yipu Liu,Yuanyuan Wu,Hui Chen,Yun Wang,Yong-Cun Zou,Dejun Wang,Xiaoxin Zou
Splitting water to produce hydrogen requires the development of non-noble-metal catalysts that are able to make this reaction feasible and energy efficient. Herein, we show that cobalt pentlandite (Co9S8) nanoparticles can serve as an electrochemically active, noble-metal-free material toward hydrogen evolution reaction, and they work stably in neutral solution (pH 7) but not in acidic (pH 0) and basic (pH 14) media. We, therefore, further present a carbon-armoring strategy to increase the durability and activity of Co9S8 over a wider pH range. In particular, carbon-armored Co9S8 nanoparticles (Co9S8@C) are prepared by direct thermal treatment of a mixture of cobalt nitrate and trithiocyanuric acid at 700 °C in N2 atmosphere. Trithiocyanuric acid functions as both sulfur and carbon sources in the reaction system. The resulting Co9S8@C material operates well with high activity over a broad pH range, from pH 0 to 14, and gives nearly 100% Faradaic yield during hydrogen evolution reaction under acidic (pH 0), neutral (pH 7), and basic (pH 14) media. To the best of our knowledge, this is the first time that a transition-metal chalcogenide material is shown to have all-pH efficient and durable electrocatalytic activity. Identifying Co9S8 as the catalytically active phase and developing carbon-armoring as the improvement strategy are anticipated to give a fresh impetus to rational design of high-performance noble-metal-free water splitting catalysts.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2022
·Vol. 97
·期 12
·3333-3343
·
IF 3.709
Yongjun Song,Aimin Wang,Songyu Ren,Yanyu Zhang,Zhenjun Wen,Zhongguo Zhang
BACKGROUND It would be highly advantageous to develop a heterogeneous electro-Fenton (HEF) system in which the catalyst is fixed to recycle easily and the electrode itself can produce and activate H 2 O 2 simultaneously. In this study, a new sandwich-like bifunctional cathode using carbon cloth (CC) loaded with FeOCl nanoparticles and activated carbon fiber (ACF) was fabricated and used in the HEF process for the degradation of antibiotic trimethoprim (TMP). RESULTS Experimental results showed that the activated carbon fiber and FeOCl-modified carbon cloth cathode (ACF/CC@FeOCl) exhibited a promising catalytic performance to reduce O 2 to generate H 2 O 2 on the surface of ACF and activate H 2 O 2 to generate hydroxyl radicals ( • OH) at the active sites of FeOCl nanoparticles, thus enabling a rapid TMP degradation in a wide pH range (3–9). Various influencing factors, such as applied cathodic current, pH and TMP concentration, were investigated, and the optimal condition was found at 0.36 A, pH 3.0, and 100 mg L −1 TMP, where 99.7% TMP was degraded within 90 min and 74.4% total organic carbon (TOC) was removed within 360 min. Under the condition of 0.36 A and initial pH 6.8, 100 mg L −1 TMP was completely degraded within 120 min and the mineralization efficiency could achieve 61.5% within 360 min. The coumarin fluorescence probing technique and radical quenching experiments revealed that • OH was the predominant reactive oxygen species (ROS) in the ACF/CC@FeOCl-HEF process. CONCLUSION The reusability and stability tests showed that the ACF/CC@FeOCl cathode has excellent performance and good stability, and this is very promising for the efficient degradation of refractory organic pollutants in the HEF process. © 2022 Society of Chemical Industry (SCI).
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2022
·Vol. 26
·期 4
·875-885
·
IF 2.747
Boakye Felix Ofori,Fan Meiling,Zhang Fangfang,Tang Haolin,Zhang Ruming,Zhang Haining
Development of transition metal phosphides with tunable morphology and chemical composition is a potential way to construct electrocatalysts with superior hydrogen evolution reaction (HER) activity in a wide range of pH values. In this work, vertical nanorods are constructed from nickel and iron phosphide grown on a carbon cloth (Ni 2 P-Fe 2 P/CC) via a hydrothermal treatment followed by low-temperature phosphorization method to achieve an effective catalyst for sufficient HER activity and strong stability. The Ni 2 P-Fe 2 P/CC exhibits remarkable overpotentials of 78, 80, and 87 mV to achieve a current density of 10 mAcm −2 in acidic, alkaline, and neutral electrolytes, respectively. Furthermore, it shows strong stability without significant performance change for 20 h, 30 h, and 30 h under 100 mAcm −2 in acidic, alkaline, and neutral electrolytes, respectively. This outstanding catalytic performance for HER in a wide pH range can be accredited to the synergistic effect induced by the coexistence of Ni and Fe atoms. Additionally, the integration of nanorods on the nanosheet also initiates fast transfer of hydrogen bubbles within the electrolyte, thereby enhancing its HER activity. The results present an opportunity to construct a low-cost, effective transition metal phosphide with unique architecture and strong durability for efficient HER activity in a wide range of pH values.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）