Journal of Environmental Sciences
·
2023
·
IF 6.9
Hanbing Meng,Shiwen Hu,Zebin Hong,Wenting Chi,Guojun Chen,Kuan Cheng,Qi Wang,Tongxu Liu,Fangbai Li,Kexue Liu,Yang Yang
Zero-valent iron (ZVI) is a promising material for the remediation of Cd-contaminated paddy soils. However, the effects of ZVI added during flooding or drainage processes on cadmium (Cd) retention remain unclear. Herein, Cd-contaminated paddy soil was incubated for 40 days of flooding and then for 15 days of drainage, and the underlying mechanisms of Cd immobilization coupled with Fe/S/N redox processes were investigated. The addition of ZVI to the flooding process was more conducive to Cd immobilization. Less potential available Cd was detected by adding ZVI before flooding, which may be due to the increase in paddy soil pH and newly formed secondary Fe minerals. Moreover, the reductive dissolution of Fe minerals promoted the release of soil colloids, thereby increasing significantly the surface sites and causing Cd immobilization. Additionally, the addition of ZVI before flooding played a vital role in Cd retention after soil drainage. In contrast, the addition of ZVI in the drainage phase was not conducive to Cd retention, which might be due to the rapid decrease in soil pH that inhibited Cd adsorption and further immobilization on soil surfaces. The findings of this study demonstrated that Cd availability in paddy soil was largely reduced by adding ZVI during the flooding period and provide a novel insight into the mechanisms of ZVI remediation in Cd-contaminated paddy soils.
研究领域:
土壤科学
·
环境修复
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Xiao-Jun Li,Shi-Jun Xiao,Yi Heng Xie,Jiang Chen,Hai-Rong Xu,Yuan Yin,Rui Zhang,Tong Yang,Tong-Yu Zhou,Si-Yan Zhang,Pei Hu,Li-Ming Gao,Hui-Ping Peng
An innovative acidic hydrolysate fingerprinting workflow was proposed for the characterization of Lyophyllum Decastes polysaccharide (LDP) by ultra performance liquid chromatography-mass spectrometry (UPLC-MS). The crude polysaccharides were firstly separated and purified by using DE-52 column and the BRT GPC purification system, respectively. The molecular weight and monosaccharide content of homogeneous polysaccharides were ascertained by utilizing HPGPC and ion chromatography separately. Secondly, the linkage of LDP was identified by methylation analysis and 1D/2D NMR spectra. The UPLC-MS/MS was used to scan and identify the acidic hydrolysate products of LDP using the PGC column. The oligosaccharides were collected by chromatography and identified by mass spectrometry. Thirdly, the expression of IL-1β, IL-6, iNOS, TNF-α and IFNAR-I was measured in order to assess the immunological activity of LDP. Besides, the targeted receptors identification of polysaccharides was performed by screening the expression of TLRs family protein. The results showed that oligosaccharide fragments with different molecular weights can be obtained by partial hydrolysis, which further verified that the structures of LDP polysaccharides was a 1–6-linked β-glucan. Moreover, the LDP polysaccharide can up-regulate the content of IL-1β, IL-6, iNOS, TNF-α and IFNAR-I and plays an important immunoregulation role through TLRs family.
研究领域:
生物化学
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免疫学
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DOI
PubMed
高影响因子
Inorganics
·
2025
·Vol. 13
·期 3
·89
·
IF 3
Bosen Zhou,Zhengbo Lai,Yuanyuan Li,Hualan Zhou,Ye Tian,Yibo Zhao,Ming Xia
The siliceous precursor was hydrolyzed from tetraethylorthosilicate (TEOS) under acidic conditions, followed by the addition of sodium aluminate and sodium hydroxide. Y zeolite was subsequently obtained through hydrothermal crystallization under alkaline conditions. Key synthesis parameters, including reactant molar ratios, crystallization temperature, and time, were systematically varied to optimize the synthesis conditions. The synthesized products were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), nitrogen adsorption analysis, and inductively coupled plasma (ICP) elemental analysis. Well-crystallized Y zeolite with a silica-alumina ratio (SAR) of 5.55 was successfully synthesized via TEOS hydrolysis catalyzed by sulfuric acid at a low crystallization temperature of 85 °C. The catalytic performance of benzyl phenyl ether, a lignin model compound, over NiY catalyst was evaluated in a high-pressure reactor. The results indicate that the catalytic efficiency of Y zeolite synthesized using TEOS as the silicon source under acidic hydrolysis conditions is significantly superior to Y zeolite prepared using alkaline silica sol as the silicon source.
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Ying Dai,Riwen Lv,Jiali Fan,Hong Peng,Zhibin Zhang,Xiaohong Cao,Yunhai Liu
Owning to highly mechanical strength and non-interference effectivity, silica dioxide is often explored as a stable supporter commonly with mesopore. It is known that a macroporous framework has larger mass transfer channel, possibly beneficial to adsorption process. Herein highly ordered macroporous silica dioxide framework (homogeneous pore size of 194.20 nm) was synthesized and embedded with supramolecular (CC/OMS). Cs cation adsorption onto CC/OMS was explored under different pH (presence or absence of humic acid), initial cesium concentration, shaking time, competing ions. The robust cesium uptake capacity demonstrated by a theory adsorption amount of 150.01 mg/g highlighted unique CC/OMS properties combining large mass transfer channel and superior complex capacity of supramolecular. The adsorption was well fit with Langmuir and pseudo-second-order model. Sodium and potassium at a lower concentration showed little influence on cesium adsorption. The results demonstrated that CC/OMS was an alternative material for cesium capture from acidic aqueous solution.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Dinghua Zhou,Min He,Yunxuan Ding,Jiaguo Yu,Ke Fan,Licheng Sun
Precious metals (like Ir, Ru, and Pt) and their derivatives are the benchmark catalysts for water splitting in acidic media due to their high stability and activity. However, the high cost and scarcity of these materials hamper the large-scale applications. To solve this issue, construction of catalysts containing low content of precious metals with high intrinsic activity can be an efficient strategy, which expectedly can decrease the cost but meanwhile preserve the activity. Herein, we synthesized an IrW/WO3 array catalyst by in situ formation of IrW alloy on hierarchical WO3 nanosheet arrays. With extremely low Ir content of 1.25 wt % in 0.5 M H2SO4, this composite catalyst not only shows superior water oxidation activity (the overpotential at 10 mA cm–2 is only 229 mV, significantly lower than that of the commercial IrO2 (358 mV)) but also exhibits excellent proton reduction performance (the overpotential at −10 mA cm–2 is 49 mV, close to that of commercial Pt/C catalyst (42 mV)), showing promising bifunctionality for the overall water splitting. As a result, only 1.5 V is needed to drive the overall water splitting at 10 mA cm–2 with a good long-term stability under acidic conditions. These remarkable features can be ascribed to the abundant active sites exposed by the three-dimensional nanostructure, and the high intrinsic activity per Ir site. The theoretical calculation verifies that Ir sites in IrW surface after oxidation have a higher intrinsic activity than IrO2 for water oxidation. We believe this research can supply a strategy to design highly active and stable catalysts with low loading of noble metals for acidic water splitting.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2024
·
IF 4.1
Boyan Ai,Guoxiang Wang,Pengchao Liang,Jinxiu Bing,Majie Zhang,Qingwang Min,Xinxin Zhang
The development of highly active and acid-stable Ru-based electrocatalysts is of great significance for water electrolysis but remains a huge challenge due to serious Ru corrosion in an acid medium. Herein, we prepared oxygen vacancy (O V )-rich Nd-doped RuO 2 nanocrystals by facile synthesis via hydrothermal and subsequent annealing for efficient overall water splitting. The catalyst exhibits an overpotential of only 200 mV for OER and 44 mv for HER at the current density of 10 mA cm −2 in 0.5 M H 2 SO 4 electrolyte. Nd-doped RuO 2 only demands a cell voltage of 1.52 V to drive the overall water splitting reaction and displays excellent stability for 100 h. Density functional theory further revealed that the newly constructed Nd-doped RuO 2 sites activate the difficult to react *O intermediates, reducing the adsorption energy of the OER intermediates to effectively minimize the Gibbs free energy (*O to *OOH) of the reaction rate-determining step and regulate the center of the active site d-band. The synergistic effect of aliovalent doping and vacancy engineering contributes to the excellent electrocatalytic performance of Nd-doped RuO 2 . This performance control strategy can pave the way for the development of effective and economically viable catalysts.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
Advanced Energy Materials
·
2024
·Vol. 14
·期 20
·2304479
·
IF 24.4
Xiaoxia Xiong,Jialin Tang,Yuan Ji,Weiqing Xue,Haoyuan Wang,Chunxiao Liu,Hongliang Zeng,Yizhou Dai,Hong-Jie Peng,Tingting Zheng,Chuan Xia,Xinyan Liu,Qiu Jiang
Proton exchange membrane (PEM) water electrolysis holds great promise in revolutionizing clean energy production by enabling the efficient generation of hydrogen. Nevertheless, a formidable challenge persists in the realm of designing electrocatalysts that are both highly active and acid-resistant during the oxygen evolution reaction (OER), thereby mitigating the substantial kinetic barrier. In this study, the facile synthesis of iridium-yttrium (IrY) alloy nanocatalysts via a thermal shock method is introduced, which exhibits exceptional activity in the context of acidic water oxidation. Through the strategic incorporation of dispersed Y into the lattice of Ir metal, the IrY catalyst demonstrates a notably low overpotential of 255 mV at a current density of 10 mA cm −2 and showcases remarkable catalytic stability in acidic electrolytes, enduring for over 500 h with a high current density of 100 mA cm −2 . Through a comprehensive set of in situ characterizations and analytical methods, the formation of a surface Ir-based oxide layer, induced by deprotonation and electrochemical oxidation is unveiled, which is notably stabilized by the presence of Y dopants. This stabilization of the active site imparts enhanced resistance to over-oxidation and dissolution, underpinning the exceptional stability of the catalyst. Theoretical calculations suggest that the incorporation of Y into the catalyst structure has a significant impact on enhancing the reactivity of the oxygen intermediate (O*) at adjacent Ir sites, thus lowering the overpotential and promoting OER activity. The alloying approach presents a straightforward method for achieving atomic-level modifications in catalyst design and can pave the way for the development of more effective and economically viable OER catalysts and beyond.
研究领域:
材料科学
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能源化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Ji Qianqian,Tang Bing,Zhang Xilin,Wang Chao,Tan Hao,Zhao Jie,Liu Ruiqi,Sun Mei,Liu Hengjie,Jiang Chang,Zeng Jianrong,Cai Xingke,Yan Wensheng
The microscopic reaction pathway plays a crucial role in determining the electrochemical performance. However, artificially manipulating the reaction pathway still faces considerable challenges. In this study, we focus on the classical acidic water oxidation based on RuO 2 catalysts, which currently face the issues of low activity and poor stability. As a proof-of-concept, we propose a strategy to create local structural symmetry but oxidation-state asymmetric Mn 4-δ -O-Ru 4+δ active sites by introducing Mn atoms into RuO 2 host, thereby switching the reaction pathway from traditional adsorbate evolution mechanism to oxide path mechanism. Through advanced operando synchrotron spectroscopies and density functional theory calculations, we demonstrate the synergistic effect of dual-active metal sites in asymmetric Mn 4-δ -O-Ru 4+δ microstructure in optimizing the adsorption energy and rate-determining step barrier via an oxide path mechanism. This study highlights the importance of engineering reaction pathways and provides an alternative strategy for promoting acidic water oxidation.
研究领域:
电化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 17
·9419-9426
·
IF 14.511
Jiabiao Yan,Jing Zhu,Dawei Chen,Shuai Liu,Xu Zhang,Shoushan Yu,Zhenhua Zeng,Luhua Jiang,Fanglin Du
Ruthenium-based pyrochlore oxides (A2Ru2O7) have emerged recently as state-of-the-art catalysts for acidic water oxidation; however, their stability still needs to be further improved. Exploring the relationship between the A-site cation and the structure of the active site (Ru) is highly desirable for designing efficient electrocatalysts. Herein, we rationally manipulate the substitution of the A-site atoms in Y2Ru2O7 (YRO) by Ho3+, which has an identical ionic radius to Y3+ but higher electronegativity due to the 4f electron effect. It was demonstrated that the higher electronegativity could enlarge the Ru–O–Ru bond angle and reduce the Ru–O bond length, mitigating the RuO6 octahedral distortion in Ho2Ru2O7 (HRO) for enhancing the intrinsic OER activity. Compared with other pyrochlore oxides, HRO displayed an ultralow overpotential of 215 mV @ 10 mA cm−2 with lower Ru content and higher mass activities, showing long-term (>60 h) stability in acid media. Density functional theory (DFT) calculations revealed that the higher electronegativity of Ho could strengthen the Ru–O covalency, thereby optimizing the free energy of oxygen species (ΔGOOH* − ΔGO2) for better catalytic activity. In addition, the higher electronegativity could reduce the oxygen vacancies and improve the formation energy of oxygen vacancies for better resistance to Ru dissolution. This work reveals the inherent relationship of the A-site atom electronegativity, the lattice structure of the active site, and the activity–stability of the catalysts.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Huiyang Bian,Maolin Dong,Lidong Chen,Xuelian Zhou,Ruibin Wang,Liang Jiao,Xingxiang Ji,Hongqi Dai
Lignocellulosic nanofibrils (LCNF) has caused great interest from researchers due to the benefits of high output, low operation cost, and weak environmental impact. The existence of lignin in LCNF can be applied to regulate the hydrophilicity and polarity, thereby endowing LCNF with unique properties. Consequently, it is crucial to tailor the production of LCNF with desirable characteristics for various applications. This work demonstrated the feasibility of on-demand regulation of lignocellulosic nanofibrils based on rapid fractionation using p-toluenesulfonic acid (p-TsOH) hydrolysis. Acid concentration of 20–80 wt %, hydrolysis temperature of 50–80 °C, and reaction duration of 20–120 min were employed to control the characteristic of reaction products. Different degrees of delignification and xylan dissolution over the entire reaction space were obtained and related to combined delignification factor (CDF) and combined hydrolysis factor (CHF), respectively. It was also found that the mean fibril height of LCNF were significantly affected by CDF and CHF, independent of each reaction process variables. Detailed characterization revealed that the resultant LCNF presented wide range of fibril height (10.6–86.4 nm) and excellent thermal stability (maximal weight loss temperature of approximately 360 °C). Overall, this work provides useful and fundamental knowledge for achieving LCNF with tailored characteristics, all of which are essential to many promising applications.
研究领域:
材料科学
·
林业工程
✓ 已验证
产品关联
DOI
高影响因子
Small Structures
·
2024
·
IF 13.9
Xiaotong Wu,Chao Lin,Weibo Hu,Chao Fu,Lei Tan,Haifeng Wang,Faiza Meharban,Xiangxiang Pan,Pan Fu,Han-Don Um,Qi Xiao,Xiaopeng Li,Miho Yamauchi,Wei Luo
Proton exchange membrane water electrolysis (PEMWE) with high-purity H 2 and O 2 products and swift response to electricity fluctuation is of great interest for renewable energy, chemical and pharmaceutical industries. Ruthenium oxide shows promise as an alternative to iridium oxide catalysts in PEMWE but suffers from severe anodic corrosion. Herein, a pluralistic electronic structure modulation approach is presented to address the instability issue of Ru, by in situ growing Mn x Ru 1− x O 2 solid solution on MnO 2 , coated carbon fibers (Mn x Ru 1− x O 2 /MnO 2 /CFs). Due to higher ion electronegativity, Mn dopants in the Mn x Ru 1− x O 2 solid solution accept electrons, activating the Ru site. Simultaneously, the MnO 2 support donates electrons to prevent Ru site overoxidation and dissolution due to its lower work function than the Mn x Ru 1− x O 2 solid solution. As a result, the Mn x Ru 1− x O 2 /MnO 2 /CFs catalyst exhibits a low overpotential of 161 mV at 10 mA cm −2 and a remarkable stability exceeding 600 h. Profiting by its improved oxygen evolution reaction (OER) kinetic activity, the Mn x Ru 1− x O 2 /MnO 2 /CF-based PEMWE shows a low cell voltage of 1.9 V at 2 A cm −2 , and stably operate at current density of 500 mA cm −2 for 24 h. This work shows the potential of the pluralistic electronic structure modulation to boost activity and stability of Ru-based acidic OER electrocatalysts.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yuhua Xie,Yumei Feng,Chen Li,Fang Luo,Qing Li,Shiao Zhu,Mingxing Gong,Zehui Yang
The industrial development of acidic water splitting significantly counts on the activity associated with stability of oxygen evolution reaction (OER) electrocatalyst. In this work, we have constructed cubic Rh@Ir core–shell for acidic water splitting. The formed Rh@Ir electrocatalyst shows a high HER performance with only 29 mV overpotential for 10 mA cm −2 , stemming from the upshifted and downshifted d band center of Ir and Rh, leading to a moderate hydrogen binding strength. The Ir atom donates its electrons to nearby Rh atoms triggering a high susceptibility in nucleophilic attack by H 2 O to generate *OOH; thereby, the overpotential required to achieve 10 mA cm −2 is 216 mV for Rh@Ir core–shell, better than commercial IrO 2 . Moreover, the stability is superior to commercial IrO 2 and pure Ir electrocatalyst due to the strong electronic interplay in Rh@Ir contributing to a better resistance towards electrochemical dissolution proved by operando Raman and electrochemical impedance spectroscopies. Only 1.55 V is needed for Rh@Ir to drive overall water splitting at 10 mA cm −2 .
研究领域:
电化学
·
材料科学
·
催化
·
能源材料
✓ 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）