CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xin Li,Jielin Wang,Jieyuan Li,Chunling Zhang,Ruimin Chen,Shujie Shen,Yanjuan Sun,Lili Zhang,Fan Dong
As one of the most important bulk chemicals, nitric acid is primarily produced by the Ostwald process with extensive energy consumption and carbon emission. Therefore, it is necessary to develop alternative green routes for nitric acid synthesis. Photocatalytic nitrate synthesis via complete ammonia oxidation is a promising strategy for efficiently producing nitrate under ambient conditions. However, the reaction route of ammonia oxidation is complex with diverse product distribution since it is a multi-electron involved reaction. It is a great challenge to directionally regulate the selectivity for the targeted conversion of ammonia into nitrate with a high conversion ratio. Herein, the CuO x clusters are constructed on the TiO 2 substrate as the active sites to facilitate ammonia-to-nitrate photosynthesis via the enhanced activation of H 2 O molecules. It is revealed that a new reaction pathway is established, in which the •OH-driven direct ammonia oxidation contributes to the promoted nitrate synthesis rate at 116.8 ± 3.5 μmol·q·h −1 . Moreover, the competitive conversion ratio for ammonia (91.1 ± 1.2 %) and selectivity for nitrate (91.7 ± 0.8 %) are reached, manifesting the significance of effective nitrate production with low energy consumption and carbon emission. A new opportunity is provided in this work for the artificial nitrogen cycle and N-involving resource utilization.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 51
·77344-77358
·
IF 5.19
Ding Baoting,Wang Xiaomeng,Feng Kun,Fu Jingran,Liang Jianru,Zhou Lixiang
Acidic Cr(VI)-containing wastewater has received increasing attention in recent years. Schwertmannite is a suitable adsorbent for its acid resistance and good adsorption ability. However, it shows poor Cr(VI) adsorption performance under acidic conditions. Herein, inspired by the fast neutralization-mineralization process of acid mine drainage (AMD) triggered by alkaline rocks, a novel nano-scaled schwertmannite (Sch-2.7) with high Cr(VI) adsorption capacity was synthesized at constant pH of 2.7 via adding OH − . Compared with common schwertmannite (Sch), appropriate OH − effectively improved mineral yield (the precipitation efficiency of Fe: 96.75% vs. 29.93%), specific surface area (65.1 m 2 /g vs. 18.9 m 2 /g), surface group content, and further Cr(VI) adsorption ability of Sch-2.7. The maximum adsorption capacity was 54.17 (pH = 3), 61.59 (pH = 4), and 66.5 mg/g (pH = 5) for Sch-2.7, whereas only 20.35, 24.51, and 27.17 mg/g for Sch. On average, the former was 2.53 times higher than the latter. Temperature and coexisting ions had little influences on the sorption process of Sch-2.7. The mechanism analysis demonstrated that the Cr(VI) removal by Sch-2.7 was a more thermodynamic favorable process due to abundant reactive-active components on Sch-2.7 for adsorption reaction. This work provided new insight into performance optimization and application potential on Cr(VI) removal of schwertmannite.
研究领域:
环境科学
·
材料科学
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PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Ying Huo,Xuyu Wang,Zebao Rui,Xiaoqing Yang,Hongbing Ji
Insight into the relationship between catalytic trends and physicochemical properties of composite nanoparticles is essential for their rational design. Herein, a series of 3d-M (M = Mn, Fe, Co, Ni) metal hydroxide-promoted PtM(OH)x/Al2O3 catalysts are developed and well characterized for establishing the catalytic HCHO oxidation reactivity trend as a function of more fundamental properties, such as hydroxyl concentration and adsorption strength. The reactivity of PtM(OH)x/Al2O3 exhibits an increasing trend of Mn < Fe < Co < Ni, which is governed by their OH–M2+δ bond strength (Ni < Co < Fe < Mn) and surface hydroxyl concentration (Mn < Fe < Co < Ni). Both PtCo(OH)x/Al2O3 and PtNi(OH)x/Al2O3 exhibit a (>)95% HCHO conversion and (>)100 h performance stability at 30 °C with a low 0.2 wt % Pt loading amount. The identification of these catalytic trends provides foundations for composite active sites design for HCHO oxidation and other hydroxyl-involved reactions.
研究领域:
催化化学
·
材料科学
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124167
·
IF 7.5
Chen Chen,Zhenyu Wang,Yasen Li,Jiayao Gao,Xin Chen,Mingjie Jia,Die Shao,Yiming Wang,Xuejian Li,Fuqiang Yu,Guangwen Xu,Junli Xu,Hong-bin Sun
Transition-metal borides have long been developed as promising electrocatalysts for the hydrogen evolution reaction (HER); however, the identity of their true active phase remains controversial. Here, in conjunction with our previous studies, by systematically investigating a series of cobalt- and nickel-boride-derived catalysts through a combined computational and experimental screening, we reveal that HER activity universally originates from the synergistic interaction between metallic sites and hydroxide matrices, enabled by lattice expansion, interfacial electronic transfer, and dynamic surface evolution. As a representative high-performance example, Pt-modified Co(OH) 2 derived from cobalt boride exhibits ultralow overpotentials of 11 mV at 10 mA cm −2 and 95 mV at 500 mA cm −2 , together with long-term stability. Importantly, the same reconstruction principle applies to Ni-boride systems, confirming the generality of this approach. Beyond water electrolysis, we further demonstrate that these HER catalysts are highly effective in Al-H 2 O batteries, where hydrogen evolution is coupled with electrical energy harvest. An alkaline Al-H 2 O battery employing the reconstructed catalyst delivers a power density of 21.96 mW cm −2 . This work establishes that the activity of “boride-based” HER catalysts fundamentally arises from reconstructed metal-hydroxide active centers, providing a development paradigm of transition-metal electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Guocui Cai,Helong Jiang,Fangyi Chu,Xiangcun Li,Xiaobin Jiang,Xiao Wu,Gaohong He,Yan Dai
Here, the conventionally disordered Co(OH)F filaments are rearranged to form highly-ordered flower-like Co(OH)F architectures in a conductive membrane substrate. The important findings contribute to designing delicate nanostructures and improving the catalytic activity of advanced materials for energy applications. The hierarchically porous CNT@NC membrane with CNT as the core and N -doped carbon as the crosslinking shell is scalably designed firstly for strengthening the transport of Li + and electrons in the electrode, providing an ultrahigh porosity for growing flower-like Co(OH)F on both surfaces and interior of the membrane, as well as offering electrons for the redox reactions through the roots of the Co(OH)F flowers. Furthermore, the ordered Co(OH)F bundles with divergent and open-ended structures provide the catalyst with the broad reaction interface and active sites for polysulfides (LiPSs) anchoring and catalytic conversion at a low energy barrier, significantly facilitating the diffusion of ions and electrolyte in the catalyst, and thus effectively alleviating the shuttle effect. Owing to the synergistic effect between the conductive membrane substrate and the grown Co(OH)F catalyst, the Co(OH)F-CNT@NC cathode generates a high reversible capacity and excellent long-term cycling performance (622 mAh·g −1 at 1C after 600 cycles). Conclusively, the proposed facile strategy provides insights regarding the design of novel cathode materials for high-areal-capacity Li–S batteries.
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高影响因子
ACS Catalysis
·
2020
·
IF 12.35
Yang Chen,Yingxin Feng,Lin Li,Jingyue Liu,Xiaoli Pan,Wei Liu,Fenfei Wei,Yitao Cui,Botao Qiao,Xiucheng Sun,Xiaoyu Li,Jian Lin,Sen Lin,Xiaodong Wang,Tao Zhang
Exclusive Pt species supported on inert substrates have not achieved satisfactory performance for cryogenic CO oxidation because of the constraint of the competitive Langmuir–Hinshelwood process in which the strongly adsorbed CO inhibits the activation of O2. Here, we develop a catalyst of Pt nanoparticles on Al2O3 that exhibits extremely high activity with 100% CO conversion at −20 °C and orders of magnitude higher specific rate than current commercial catalysts. Detailed catalyst characterizations reveal the presence of metallic Pt sites and positively charged ones associated with the OH species in Pt/Al2O3. Both experimental data and theoretical calculations suggest that CO adsorbed on Pt(OH) kink sites reacts with OH species covering Pt0 terrace sites to release CO2. Afterward, O2 is facilely activated on terrace sites to regenerate OH. The presence of OH species and the synergy between Pt kink and terrace sites on the Pt species lead to an ultralow reaction barrier for CO oxidation.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Li Zou,Jiale Xie,Shuxiang Wang,Yixing Yu,Jing Huang,Liuliu Wang,Pingping Yang,Wenyan Tao
Low charge separation efficiency ( η sep ) of TiO 2 impedes its applications of photoelectrochemical (PEC) water splitting. A positive potential pretreatment approach has been developed to construct a surface polarization with −OH groups at a potential of 1.48 V RHE . When the pretreatment time of 6 h is used, the η sep and photocurrent density ( J ph ) reach up to 54% (vs. 24%, TiO 2 ) and 0.92 mA cm −2 (vs. 0.32 mA cm −2 , TiO 2 ) under AM 1.5 G illumination, respectively. The photovoltage can be increased from 0.17 V to 0.52 V. When the pretreatment time is extended to 22 h, a higher J ph of 1.57 mA cm −2 and η sep of 87% can be obtained. Furthermore, the positive potential pretreated TiO 2 possesses excellent PEC stability. The PEC improvements can be attributed to the surface polarization with the −OH groups and favorable surface states of Ti-OH, but not to the formation of Ti 3+ or oxygen vacancies.
研究领域:
材料科学
·
能源科学
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DOI
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Shidong Song,Junjie Ma,Huanlei Zhao,Phumlani F. Msomi,Jiahao Ren,Yanan Liu,Run Ma,Wanyu Ye
In terms of stability and safety, quasi-solid-state lithium-oxygen batteries (QSSLOBs) outperform traditional liquid LOBs. However, using redox mediators (RMs) in QSSLOBs requires unique strategy to inhibit the shuttle effect of RMs. In this work, a PEO-based oxygen electrode with anchored 4-OH-TEMPO (4-hydroxy-2,2,6,6-tetramethyl-piperidinyloxy) RM (referred to as TEMPO-PEO) is developed via hydrogen-bonding interaction for QSSLOBs. The TEMPO-PEO oxygen electrode can perform both significant mediation function and oxygen reduction reaction (ORR) activity. The QSSLOB using TEMPO-PEO electrode achieves a low discharge/charge voltage gap of 0.9 V and a high Coulombic efficiency of 96.8 %, which is significantly superior to the counterparts using TEMPO solution (TEMPO cell) or unanchored TEMPO (TEMPO+PEO cell). On this basis, the TEMPO-PEO cell achieves an unprecedented cycle performance for 320 cycles under the limited capacity of 300 mAh g −1 , overwhelmingly outperforming the counterpart cells that only deliver 63 cycles (TEMPO cell) and 119 cycles (TEMPO+PEO cell), respectively. After cycling, the TEMPO RM can still be well retained on TEMPO-PEO oxygen electrode and no significant side product is formed on the after-cycled Li anode of TEMPO-PEO cell, explicitly demonstrating a strong and consistent anchoring effect on suppressing the shuttling of RM species.
研究领域:
材料科学
·
电化学
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高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Yulan Song,Cuilan Tang,Tao Wang,Yansong Liu,Xiaoshan He,Chunping Xie,Guo Chen,Chengfu Deng,Zhibing He,Jinglin Huang
Constructing electronic structures with abundant surface/interface structures and effective regulation of catalytic active centers is an effective strategy to improve electrocatalytic performance, but designing efficient bifunctional non-noble metal oxygen evolution reaction (OER) and urea oxidation reaction (UOR) electrocatalysts remains challenging. Studies have shown that p-n heterojunctions can effectively regulate the electronic structure of catalytic active sites while having abundant surface/interface structure, which plays an important role in improving the native catalytic activity. Herein, FeNi-OH/Co(OH) 2 /NF p-n heterojunction structure was constructed by a simple electrochemical deposition method, and the effects of content, deposition time, and number of cycles on catalytic performance were investigated. The results show that Fe(0.02 M)Ni(0.07 M)–OH(100 s)/Co(OH) 2 (5)/NF composite material has the best OER and UOR catalytic performance. For OER, the electrocatalyst only requires an overpotential of 271 mV to obtain a current density of 50 mA cm −2 , and an applied voltage of 1.56 V to obtain a total water decomposition of 10 mA cm −2 (FeNi-OH/Co(OH) 2 /NF||Pt). For UOR, a voltage of only 1.314 V ( vs. RHE) is required to achieve a current density of 10 mA cm −2 , and an applied voltage of 1.44 V can achieve a current density of 10 mA cm −2 . Experimental, in situ measurements and theoretical results indicate that the improvement in catalytic activity is mainly due to the potential difference between FeNi-OH and Co(OH) 2 , which induces self-driven charge transfer at the interface, promoting the adsorption of reactant molecules, optimizing reaction barriers, accelerating chemical bond cleavage, and thus promoting catalytic reactions.
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Nutrition & Metabolism
·
2022
·Vol. 19
·期 1
·1-9
·
IF 4.654
Qiu Fubin,Li Rui,Gu Siyu,Zhao Yimin,Yang Linxue
Background Iron and vitamin D (VD) is essential to health. Previous studies have shown that iron homeostasis has a potential effect on VD metabolism, but the mechanism is not fully understood.ObjectivesTo explore the relationship between VD metabolism and iron metabolism, as well as the regulatory mechanism of iron on VD metabolism.Methods 40 male rats were fed adaptively for 7 days and randomly divided into control (C, n = 6 normal diet) group and model (M, n = 24 iron deficient diet) by simple randomization, the latter was used to establish iron deficiency anemia (IDA) model. After 6 weeks of feeding, the M group was randomly divided into: iron deficiency group (DFe), low iron group (LFe), medium iron group (MFe) and high iron group (HFe) by block randomization. Different doses of iron dextran (based on iron content (100 g·bw·d)): 0, 1.1, 3.3 and 9.9 mg) were given respectively. After 4 weeks, the rats were anesthetized with 8% chloral hydrate, Blood (collected from the abdominal aorta), liver and kidney tissues were collected. The serum and tissues were separately packed and frozen at -80℃ for testing.Results The results showed that the levels of hemoglobin (Hb), red blood cell (RBC), serum iron (SI), liver iron, and kidney iron in DFe group were lower than those in the other four groups, while the levels of total iron-binding capacity (TIBC), transferrin (TF) and transferrin receptor (Tfr) in DFe group were higher than those in other groups; The serum levels of 25-(OH)D3 and 1,25-(OH)2D3 in DFe group were significantly lower than those in C group (P < 0.05). The correlation analysis showed that the levels of 25-(OH)D3 and 1,25-(OH)2D3 were negatively correlated with TIBC, TF and Tfr no correlation with SI. Western blotting, immunofluorescence, and q-PCR results showed that compared with C group, the protein and gene expressions of CYP2R1, CYP27A1, and CYP24A1 in DFe group were down-regulated, and the expression of CYP27B1 protein and gene was up-regulated in DFe group.Conclusion Iron may be involved in the metabolism of VD3 by regulating the expression of VD3 hydroxylase, suggesting that appropriate iron supplementation might promote the activation of VD3.
研究领域:
营养学
·
生物化学
·
药理学
·
动物生理学
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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Siqi Liu,Xiezhen Zhou,Weiqing Han,Jiansheng Li,Xiuyun Sun,Jinyou Shen,Lianjun Wang
Flutriafol is one of the widely used triazole fungicides in global pesticides market, and its degradation mechanisms are important to develop powerful technologies to remove it. Insight into the kinetics and mechanisms of · OH-mediated mineralization of flutriafol have been obtained using quantum chemical calculation and electrochemical experiment methods. The complete · OH-mediated degradation pathway of flutriafol was proposed by density functional theory (DFT) simulation and the potential energy surface was mapped out for possible reactions. On the basis of DFT calculations, the optimal · OH-mediated mineralization mechanism of flutriafol was revealed, and a series of intermediates were observed accumulated in the degradation process, most significance among which were (2-fluorophenyl) (4-fluorophenyl)-Methanone, phenol , dihydroxybenzenes, benzoquinones , muconic acids , maleic acids , oxalic acids and formic acid . To give deeper insight into the · OH-mediated reaction mechanism, the electrostatic potential (ESP) and average local ionization energy (ALIE) analysis were conducted for o-benzoquinone and p-benzoquinone. The proposed mechanism was further validated by electrochemical experiments at TiO 2 -NTs/SnO 2 -Sb/PbO 2 anode. The main intermediates were identified and quantified by experimental method, indicating that the proposed · OH-mediated degradation mechanism derived from DFT calculations was feasible. These detailed findings could be instrumental for a comprehensive understanding of the · OH-mediated mineralization mechanism of flutriafol and the similar contaminants.
研究领域:
环境科学
·
化学
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DOI
高影响因子
Journal of Energy Storage
·
2026
·
IF 10.7
Yongbo Liu,Yang Chen,Limei Song,Jianhua Gao
In the field of electrochemical energy storage, polyanionic compounds exhibit outstanding electrochemical performance owing to their stable crystal structures and tunable operating potentials. Among these, vanadium-based phosphates stand out and have been extensively investigated. In this work, a novel polyanionic compound, Na 3 V(OH)(HPO 4 )(PO 4 ), was synthesized by a simple one-step hydrothermal method. Its crystal structure, confirmed by Rietveld refinement of the X-ray diffraction data, can accommodate sodium ions and provide open interstitial pathways to facilitate Na + diffusion, suggesting its potential as a cathode material for sodium-ion batteries (SIBs). Bond valence sum analysis and density functional theory calculations further validated the high Na + ion transport efficiency within the framework. Based on these findings, a half-cell was assembled using the as-prepared material as the cathode and metallic sodium as the anode. Electrochemical tests demonstrated excellent reversible cycling stability and rate capability, underscoring the promise of Na 3 V(OH)(HPO 4 )(PO 4 ) as a high-performance cathode candidate for SIBs.
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