Journal of Cleaner Production
·
2025
·
IF 10
Ziheng Han,Xiude Hu,Qiuyan Xue,Tuo Guo,Jingjing Ma,Qingjie Guo
The current challenge in the advancement of chemical looping ammonia synthesis (CLAS) technology lies in the poor reaction efficiency of binary transition metal nitrogen carriers (NC), which are limited to a single type. A new type of VN NC modified through the doping with transition metals (Ni, Fe, Co) has been investigated. The loading of Ni, Co and Fe significantly enhances the capability of VN to catalyze the dissociation of H 2 and increased the quantity of surface nitrogen vacancies (Nv), thereby promoting the transformation of nitrogen lattice to produce NH 3 . Theoretical calculation indicated that the presence of Ni is also indicative of its role in promoting the decomposition of H 2 and improving the affinity of lattice nitrogen for H*. The addition of 25 wt% Ni as a dopant has a pronounced activation effect on the VN. This results in a substantial increase in the lattice nitrogen conversion rate from 3.3% to 49.2%. The rate of ammonia production escalated from 30.5 μmol g −1 ·h −1 to 508 μmol g −1 ·h −1 . The Ni-VN demonstrates a sustained selectivity of 87% towards NH 3 at 850 °C. After conducting 8 cycles of experiments, it was observed that the activity of Ni-VN did not exhibit a significant decrease. This study offers a novel viewpoint on the advancement and formulation of transition metal-based NC, which contributes to the progress of low-carbon, environmentally friendly synthetic ammonia technology.
研究领域:
化学工程
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材料科学
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催化化学
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产品关联
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 8
·1809
·
IF 4.2
Yuhong Zhao,Qi Zhang,Zhuhua Gong,Wenlin Zhang,Yun Ren,Qiang Li,Hongjia Lu,Qinhong Liao,Zexiong Chen,Jianmin Tang
In this study, we prepared high-nitrogen self-doped porous carbons (NPC1 and NPC2) derived from the pruned branches and seeds ofZanthoxylum bungeanumusing a simple one-step method. NPC1 and NPC2 exhibited elevated nitrogen contents of 3.56% and 4.22%, respectively, along with rich porous structures, high specific surface areas of 1492.9 and 1712.7 m2g−1and abundant surface groups. Notably, both NPC1 and NPC2 demonstrated remarkable adsorption abilities for the pollutant methylene blue (MB), with maximum monolayer adsorption capacities of 568.18 and 581.40 mg g−1, respectively. The adsorption kinetics followed the pseudo-second-order kinetics and the adsorption isotherms conformed to the Langmuir isotherm model. The adsorption mechanism primarily relied on the hierarchical pore structures of NPC1 and NPC2 and their diverse strong interactions with MB molecules. This study offers a new approach for the cost-effective design of nitrogen self-doped porous carbons, facilitating the efficient removal of MB from wastewater.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
PubMed
高影响因子
Materials Today Communications
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2021
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IF 3.383
Shijiao Zhao,Rui Xu,Jingtao Ma,Changsheng Deng,Xing Cheng,Xingyu Zhao,Shaochang Hao,Jianjun Li
Zirconium nitride is an increasingly attractive material, owning to its wide range of applications. Nitridation with carbon as a reductant is a commonly used process for the preparation of transition metal nitrides. In this study, the nitridation of carbon-containing zirconia gels was studied as a method to synthesize zirconium nitride. The behavior of the gel upon heat treatment was investigated online. The evolution of the microstructure during nitridation was investigated using high-resolution transmission electron microscopy (HRTEM). The relationships between the gaseous species, crystalline phases, microstructure, and chemical elements of the resulting materials were established. The results showed that NH 3 , CH 2 O, CO 2 , CO, H 2 O, and HCN were the gaseous products in the nitridation process. Nucleation of the nanograins started with zirconium oxynitride . Transformation from oxynitride to nitride led to the occurrence of open-mouth-like defects on the particles. The enrichment of N atoms was accompanied by a core-shell structure. Finally, a systematic nitridation mechanism involving five stages was proposed. This study is important for understanding the nitridation process and controlling the structure and properties of transition metal nitrides.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Caihong Wang,Weiliang Qi,Ying Zhou,Wandi Kuang,Tamil Azhagan,Tiju Thomas,Chunjie Jiang,Siqi Liu,Minghui Yang
Efficient semiconductor-cocatalyst junctions are of direct relevance to solar energy based fuel generation. Here, Ni-Mo ternary nitrides based one-dimensional hierarchical structures (In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni)) have been successfully prepared and used to achieve visible light driven H 2 evolution. Because of the metallic-like properties of the transition metal nitrides, Ni 0.2 Mo 0.8 N(Ni) as co-catalysts can promote photo-generated charge-carriers transportation/separation and decrease the overpotential of H 2 -evolution. Thus, the photocatalytic property of optimal 1 wt% In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni) exhibits a hydrogen evolution rate of 614.2 μmol g -1 h −1 , which is about 10 times as high as that of blank In 2 S 3 (61.4 μmol g −1 h −1 ). Besides, the pure Ni 0.2 Mo 0.8 N shows higher co-catalytic properties than Ni 0.2 Mo 0.8 N(Ni). This indicates that the metallic Ni (and related species) lowers the co-catalytic role of ternary nitrides. Another robust indication of this is the fact that In 2 S 3 -Ni 0.2 Mo 0.8 N nanohybrid displays about 2 times higher H 2 evolution rate than In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni).
研究领域:
材料科学
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能源化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Yudong Zhang,Yuan He,Jun Li,Yang Xu,Yang Yang,Yao Ge,Xun Zhu,Qiang Liao
Optimizing non-noble catalysts for the oxygen reduction reaction (ORR) is crucial for advancing energy storage and conversion technologies. This study investigates the influence of iron valence states and nitrogen precursor contents on the physicochemical properties and electrochemical performance of lignin-based Fe–N–C catalysts. Catalysts are synthesized using different valence iron sources and varying pyrrole contents. The results reveal that iron(II) doping increases microporosity and specific surface area, while iron(III) doping enhances mesoporous and iron contents of the carbon materials. XPS and Raman spectroscopy confirm the successful incorporation of Fe–Nx active sites in the as-prepared LFeIIIPx catalysts. Electrochemical tests demonstrate that LFeIIIP10 exhibits the highest ORR activity, surpassing commercial Pt/C in half-wave potential (E1/2) and limiting current density (JL). The direct formate fuel cell (DFFC) with an LFeIIIP10 air cathode achieves a maximum power density of 24.7 mW cm–2, 32% higher than that with a Pt/C cathode. This study highlights the critical role of tailoring iron valence states and nitrogen levels to develop high ORR performance, cost-effective Fe–N–C catalysts, providing valuable insights for the future design of non-noble metal catalysts in energy applications.
研究领域:
材料科学
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能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PEDOSPHERE
·
2023
·
IF 5.7
Feng WANG,Jing ZHANG,Yanqiong ZENG,Honghui WANG,Xiyu ZHAO,Yilin CHEN,Huanhuan DENG,Liyun GE,Randy A. DAHLGREN,Hui GAO,Zheng CHEN
Elevated arsenic (As) mobilization and increased nitrous oxide (N 2 O) emission are two primary environmental concerns existing in flooded paddy soils. In this study, dissolved As(III), N isotope-labeled Na 15 NO 3 , and/or 14 NH 4 Cl were incorporated into a microcosm incubation to determine the effects of N fertilization regimes on As mobilization and N 2 O emission in a flooded paddy soil. Because nitrate had a higher redox potential and comprised a higher proportion of N substrate, As(V) was preferentially formed due to enhanced nitrate-dependent microbial As(III) oxidation. Thus, As availability was correspondingly attenuated due to the improved production of less mobile and toxic As(V). After 2-d incubation, more than 90% and 98% of soluble As(III) were immobilized in the As + NH 4 + -N + NO 3 - -N and As + NO 3 - -N treatments, respectively. Following nitrate depletion (after 2 d), microbial As(V) and Fe(III) reductions were gradually enhanced, which was attributed to stimulation of anaerobic ammonium oxidation (anammox) coupled to Fe(III) reduction, known as Feammox, by the abundance of NH 4 + . By the end of the incubation period (10 d), the As + NO 3 - -N treatment led to higher As immobilization of originally added As(III) ( ca . 61%) than the As + NH 4 + -N + NO 3 - -N treatment (42%). The As + NH 4 + -N + NO 3 - -N treatment prominently mitigated N 2 O emission compared to the As + NO 3 - -N treatment, which was ascribed to anammox, inducing accumulation of byproducts from incomplete denitrification. High-throughput sequencing indicated that the relative abundances of denitrifiers ( e.g ., Azoarcus , Ochrobactrum , and Thiobacillus denitrificans ) increased in the As + NO 3 - treatment, whereas quantitative polymerase chain reaction results indicated higher 16S rRNA gene copy numbers for anammox and Feammox (Acidimicrobiaceae bacterium A6) bacteria in the As + NH 4 + + NO 3 - treatment. Collectively, the experimental results demonstrated that N fertilization can be a feasible As remediation strategy while providing an effective strategy for mitigating N 2 O emission from paddy soils at the same time.
研究领域:
环境科学
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土壤学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2018
·Vol. 44
·期 7
·8710-8715
·
IF 3.057
Yang Chen,Chengji Deng,Chao Yu,Jun Ding,Hongxi Zhu
ZrN nanopowders were obtained by using ZrO 2 and Mg as the main raw materials in a molten salt environment and a high-purity nitrogen atmosphere. The effects of ZrO 2 / Mg mole ratio, nitriding temperature , and holding time on the synthesis of ZrN were investigated. ZrN was formed at 700 °C for 3 h. When the nitriding temperature increased to 1000 °C, pure phase ZrN was formed. The specific surface area of ZrN was 20.92 m 2 /g. When the temperature rose to 1100 °C, the resulting ZrN particles were finer; the average size of ZrN decreased from 71.60 to 49.65 nm. Further, an excessively long holding time led to evaporation of the molten salt, ZrO 2 , which was not fully nitrided. Finally, a possible formation mechanism of ZrN is proposed.
研究领域:
材料科学
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无机化学
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纳米材料
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高温合成
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Jingzhu Zhou,Qiong Qu,Wenwen Zhang,Hongyu Wang,Dongsheng Zhang,Guihua Liu
The inherent volume expansion of sulfur, the low conductivity of sulfur species, and the shuttle effects of lithium polysulfides (LiPSs) have limited the commercial deployment of lithium–sulfur (Li–S) batteries. Herein, a tungsten oxynitride skeleton featured with a three-dimensional ordered macroporous (3DOM) structure and embedded with ZIF-67-derived Co-NC nanoparticles (S/Co-NC/WNO) is developed as an effective sulfur host in Li–S batteries. The stable and unique 3DOM structure is conducive to electrolyte permeation and reduces the influence of the volume expansion. Nitrogen doping not only enhances the electrical conductivity of WO3 but also favors LiPS trapping. Meanwhile, Co-NC nanoparticles act as catalytic centers, promoting LiPS adsorption and catalytic conversion, leading to quick and durable Li–S chemistry. Therefore, S/Co-NC/WNO exhibits outstanding electrochemical performance. The initial discharge capacity is 1028.5 mAh g–1 at 0.2 C, and after 100 cycles, a discharge capacity of 938.0 mAh g–1 is maintained. Even under a sulfur loading of 8 mg cm–2, the Li–S battery was capable of reaching an areal capacity of 5.54 mAh cm–2. In addition, the flexible pouch cell based on S/Co-NC/WNO cathode also achieved stable cycling performance, which demonstrates its promising potential in Li–S battery applications.
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
Animal Nutrition
·
2025
·
IF 7.5
Zhanbo Xiong,Xiaoyin Zhang,Shiqi Zhang,Kexin Li,Yuan Gao,Ying Bu,Nan Zheng,Shengguo Zhao,Jiaqi Wang
Reducing nitrogen loss and improving nitrogen utilization efficiency in dairy cows can reduce economic costs and mitigate the environmental impact of nitrogen emissions. Red clover isoflavone, a natural compound derived from plant extract, has the advantage of biological safety. This study aimed to investigate the effects of red clover isoflavone on lactation performance and nitrogen metabolism in dairy cows. Sixty-eight Holstein cows (165 ± 21 d in milk, 710 ± 75 kg initial body weight, 2.30 ± 1.21 parities, 33.93 ± 3.81 kg/d milk yield) were chosen in a randomized complete block design. Cows were divided into 5 blocks by milk yield and randomly assigned to 4 treatments (17 cows per treatment). The experimental period lasted 84 d, during which cows were fed a basal diet supplemented with red clover extract (RCE) at 0, 2, 4, or 8 g/kg of total mixed rations (TMR) on a dry matter (DM) basis. These levels corresponded to red clover isoflavones of 0, 0.46 (0.31 g/kg formononetin and 0.15 g/kg biochanin A), 0.93 (0.67 g/kg formononetin and 0.26 g/kg biochanin A), and 1.83 g/kg (1.32 g/kg formononetin and 0.52 g/kg biochanin A), respectively. With increasing supplementation of RCE in TMR, milk yield increased quadratically by 4.65% to 9.64% ( P = 0.020) and feed efficiency improved by 6.58% to 10.53% ( P = 0.005), with the optimal dose identified as 2 g/kg. Additionally, RCE supplementation significantly increased the yield of milk components, including fat, protein, lactose, non-fat milk solid, and total milk solid ( P < 0.05), with the highest in the 2 g/kg group. Regarding nitrogen metabolism, RCE supplementation linearly increased microbial nitrogen (MN) from 782.61 to 956.41 g/d ( P = 0.003), which was accompanied by a linear increase in nitrogen utilization efficiency from 26.32% to 30.31% ( P < 0.001). In contrast, urinary total nitrogen ( P = 0.027) and milk urea nitrogen ( P < 0.001) decreased quadratically with increasing doses of RCE, reaching their minimum at 4 g/kg. Following RCE supplementation, the apparent digestibility of DM, organic matter (OM), and neutral detergent fiber (NDF) exhibited a quadratic effect ( P < 0.05), with significantly higher digestibility observed in the 2 g/kg group. Metabonomics results revealed that RCE supplementation significantly upregulated the top 12 differential metabolites. These findings suggest that RCE supplementation at levels ranging from 2 to 4 g/kg DM enhances lactation performance, milk quality, and nitrogen metabolism in dairy cows.
研究领域:
动物营养学
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乳品科学
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代谢学
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植物化学
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环境生理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIOMASS & BIOENERGY
·
2025
·
IF 5.8
Dong-hong Nan,Cheng-bo Zhang,Qi Niu,Shi-yu Feng,Bin Hu,Ji Liu,Kai Li,Qiang Lu
Nitrogen-doped activated carbon (NAC) has shown great potential in selectively catalyzing the pyrolysis of biomass to produce alkoxyphenols, with the structural characteristics being key to influencing alkoxyphenol yields. In this study, a method for preparing nitrogen-doped hydrothermal carbon (HY-NAC) by hydrothermal carbonization coupled with ammonia water activation was proposed. The resulting carbon was then used as catalyst in the selective preparation of alkoxyphenols by catalytic pyrolysis of biomass, with the 9,10-dihydroanthracene (DHA) being selected as the hydrogen donor. The physical and chemical properties of HY-NAC were systematically studied. Based on the pyrolysis-gas chromatography/mass spectrometry, the effects of the carbonization method and ammonia concentration during HY-NAC preparation, and the pyrolysis temperature, catalyst/pine ratio, and DHA/pine ratio during the pyrolysis process on the yields of alkoxyphenols were investigated. The results showed that, compared to the activated carbon prepared by pyrolytic carbonization method, HY-NAC had a larger specific surface area, higher nitrogen content, and higher contents of pyridinic nitrogen and pyrrolic nitrogen, thus exhibiting stronger catalytic performance. At an ammonia concentration of 10 %, the specific surface area of HY-NAC was 947.488 m 2 /g, and the relative contents of pyridinic nitrogen and pyrrolic nitrogen were 38.04 % and 33.22 %, respectively. Under pyrolysis temperature of 500 °C, HY-NAC/pine ratio of 3:1, and DHA/pine ratio of 1:1, the alkoxyphenol yield reached the maximum of 7.42 wt%.
研究领域:
催化化学
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生物质转化
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材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
DIAMOND AND RELATED MATERIALS
·
2024
·
IF 4.3
Yu Wang,Yanling Wang,Yunmei Du,Yanru Liu,Volodymyr Turkevych,Lei Wang
Transition metal nitrides (TMNs) have attracted great attention as ideal active materials in the field of electrocatalysts in recent years due to their excellent electrical conductivity, wide band gap and adjustable morphology. Pure phase Co 4 N nanoparticles encapsulated nitrogen-doped carbon (NC) nanotubes (Co 4 N@NC) were in-situ synthesized by one-pot method. In this paper, the morphology of carbon nanotubes is controlled by adjusting the pyrolysis time, so that more active sites are exposed on carbon nanotubes. Thus, the cobalt nitride catalyst with excellent catalytic performance for hydrogen evolution reaction (HER) in acidic electrolyte was obtained. In summary, due to the protection of mesoporous nitrogen-doped carbon to Co 4 N nanoparticles, large electrochemically active surface area, good conductivity and more exposed active sites, Co 4 N@NC possesses excellent HER performance in acidic electrolytes. The overpotential of Co 4 N@NC at the current density of 10 mA cm −2 is 117 mV (η 10 ), and it shows long-term stability in 0.5 M H 2 SO 4 solution for 50 h. This study provides a strategy for the development of catalysts for the controllable synthesis of high-performance transition metal nitrides.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Zishui Dong,Sinuo Li,Eldon R. Rene,Yixuan Liu,Weifang Ma
2,4,6-Trichlorophenol (2,4,6-TCP) is commonly used in the production of insecticides and preservatives with the characteristics of accumulation and toxicity due to the complex chemical structure with a halogenated aromatic ring. In order to effectively degrade and mineralize 2,4,6-TCP from water, a stack-coral-like catalyst of magnetic sulfur doping constructed nitrogen vacancies in graphitic carbon nitrides (Fe 3 O 4 /S-g-C 3 N 4 , FSCN-T) was designed and prepared through polymerization combined with precipitation. This visible-light-driven photocatalytic degradation to 5 mg/L 2,4,6-TCP was 95 % within 60 min with 0.1 g/L FSCN-T amendment. The degradation and carbonization rate constant were 0.118 and 0.089 min −1 respectively. This high removal was attributed to nitrogen vacancies, which broaden the visible light absorption range and shorten the electron transfer path with narrow CN bandgap (from 2.94 eV to 2.49 eV). Moreover, the introduction of iron accelerated electron cycling and enhanced magnetic recovery performance with above 95 % recovery and catalytic stability after 5 cycles of use. The degradation contribution from the active species were h + (41 %)> •OH (28.9 %) > •O 2 - (16.1 %)> 1 O 2 (8.7 %). This degradation underwent three pathways of substitution, elimination, and hydroxyl oxidation. Further, the intermediates were oxidized with ring opening and mineralization according to density functional theory (DFT) calculations and LC-Qtof-MS identification. The oxidative degradation process reduced the toxicity of 2,4,6-TCP and its intermediates. This study provided an efficient catalyst and low-energy consumption approach for toxic wastewater treatment.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子