PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
·
IF 6.9
Shuoshuo Feng,Xufeng Rao,Xiaoyu Chen,Fanghua Ning,Min Wang,Yuyu Liu
The electrocatalytic reduction of nitrate offers an environmentally friendly means of eliminating hazardous nitrate from wastewater while simultaneously yielding ammonia, a vital fertilizer precursor. Given the importance of nitrate reduction for environmental remediation and the potential of electrochemical methods, the development of a highly efficient and selective electrocatalyst specifically for nitrate reduction to ammonia (NO 3 ER) is crucial. The Cl-doped Co 4 S 3 (Cl-Co 4 S 3 ) catalyst was successfully synthesized via a solvothermal method in methanol, aiming to enhance nitrate electroreduction. The incorporation of chlorine was found to modulate the local electronic environment around cobalt atoms, enhancing their reactivity and leading to exceptional catalytic performance for nitrate reduction, leading to exceptional catalytic performance. At an operating potential of −0.61 V vs. the reversible hydrogen electrode, Cl-Co 4 S 3 exhibited remarkable Faradaic efficiency (97.64 ± 2.03 %) and yield rate (0.652 ± 0.012 mmol h −1 cm −2 ) for ammonia production, surpassing the majority of reported electrocatalysts for NO 3 ER.
研究领域:
环境科学
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材料科学
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电化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Qiufan Sun,Yuxiang Zhu,Yan Wang,Zhengtao Jia,Xiang Zhong,Jianfeng Yao
Three isostructural MIL-68(M)-NH 2 frameworks (M = In, Fe, or Al) featuring different metal centers were synthesized to investigate their photocatalytic activities for nitrogen fixation. The influence of the metal oxo clusters on the crystalline structures, morphologies, and optical characteristics was examined. MIL-68(In)-NH 2 (MNI) with one-dimensional microrod structures has a larger surface area than bulk MIL-68(Fe)-NH 2 (MNF) and spherical MIL-68(Al)-NH 2 (MNA), and achieves an ammonia generation rate (140.34 μmol g cat −1 h −1 ) ca . 3.4 and 1.6 times higher than those of MNF (37.25 μmol g cat −1 h −1 ) and MNA (87.5 μmol g cat −1 h −1 ), respectively. The superior performance can be attributed to its high crystallinity, strong coordination between the In−oxo clusters and ligands, and microrod morphology, which enhance electron transfer, improve mass transport, and extend visible light absorption. Moreover, MNI shows greater stability in ethanol aqueous solution than other sacrificial reagents, such as methanol, potassium sulfite, and triethanolamine. While slight surface corrosion of the microrods occurs in methanol and potassium sulfite solutions, complete collapse is observed in triethanolamine.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 14
·3566-3575
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IF 6.569
Libo Wang,Mohan Li,Qiu Zhang,Fengyan Li,Lin Xu
Global warming has caused us to seek a sensible strategy to replace the energy consumption of the Haber–Bosch approach in manufacturing ammonia. NH3 is utilized in agriculture to produce fertilizer to gratify the rapid increase of human food demand. Herein, we report the construction of a heterojunction that adopted g-C3N5 and Fe3+-doped W18O49 (Fe-W18O49) for photocatalytic nitrogen fixation for the first time. The surface of g-C3N5 was porous and fluffy, and its band gap energy was relatively narrow, which could adjust the absorption range of the hybrid and improve the utilization efficiency of light energy. Fe-W18O49 nanowires were rich in oxygen vacancies (OVs) that provided sufficient active sites for nitrogen adsorption and activation. The generated complex had excellent electron and hole separation ability, and the photogenerated carriers were successfully distributed to two different substances, which significantly elevated the nitrogen fixation capacity of the catalyst. The formation rate of ammonia reached 131.6 μmol g−1 h−1 when Fe-W18O49/g-C3N5 was employed as the catalyst for nitrogen fixation, which was obviously enhanced as compared with pure g-C3N5 or Fe-W18O49. This has provided the possibility to construct an inexpensive nitrogen fixation catalyst with outstanding catalytic properties.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
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2021
·Vol. 132
·期 2
·1211-1224
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IF 2.081
Zhang Long,Ge Jianhua,Zhuang Tao,Ding Xiulong,Zheng Xuyang
A series of novel sodium persulfate (Na 2 S 2 O 8 ) modified g-C 3 N 4 photocatalysts were prepared in this study to enhance nitrogen fixation. Characterization results found that the type of precursors and the mass ratio affect the crystal structure, morphology, and optical properties of the modified g-C 3 N 4 . The photocatalysts exhibited considerable nitrogen vacancies (N Vs ) depending on the nature of the different precursors and their mass ratios to Na 2 S 2 O 8 . In addition, the production rate of ammonia of the modified g-C 3 N 4 was significantly higher than that of pure g-C 3 N 4 under optimal conditions. The four cycles show modified g-C 3 N 4 excellent stability. Combined with the results of pH test, the possible mechanism of the photocatalytic nitrogen fixation process using modified g-C 3 N 4 was proposed.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Science Bulletin
·
2019
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IF 6.277
Xiang Gao,Li An,Dan Qu,Wenshuai Jiang,Yanxiao Chai,Shaorui Sun,Xingyuan Liu,Zaicheng Sun
Photocatalytic N 2 fixation involves a nitrogen reduction reaction on the surface of the photocatalyst to convert N 2 into ammonia. Currently, the adsorption of N 2 is the limiting step for the N 2 reduction reaction on the surface of the catalyst. Based on the concept of photocatalytic water splitting, the photocatalytic efficiency can be greatly enhanced by introducing a co-catalyst. In this report, we proposed a new strategy, namely, the loading of a NiS co-catalyst on CdS nanorods for photocatalytic N 2 fixation. Theoretical calculation results indicated that N 2 was effectively adsorbed onto the NiS/CdS surface. Temperature programmed desorption studies confirmed that the N 2 molecules preferred to adsorb onto the NiS/CdS surface. Linear sweep voltammetry results revealed that the overpotential of the N 2 reduction reaction was reduced by loading NiS. Furthermore, transient photocurrent and electrochemical impedance spectroscopy indicated that the charge separation was enhanced by introducing NiS. Photocatalytic N 2 fixation was carried out in the presence of the catalyst dispersed in water without any sacrificial agent . As a result, 1.0 wt% NiS/CdS achieved an ammonia production rate of 2.8 and 1.7 mg L −1 for the first hour under full spectrum and visible light ( λ > 420 nm), respectively. The catalyst demonstrated apparent quantum efficiencies of 0.76%, 0.39% and 0.09% at 420, 475 and 520 nm, respectively. This study provides a new method to promote the photocatalytic efficiency of N 2 fixation.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
MATERIALS RESEARCH BULLETIN
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2021
·
IF 4.641
Xinshan Rong,Shixian Zhang,Jian Rong,Jing Wei,Xuchun Qiu,Zhiren Wu
Z-scheme nitrogen-deficient graphitic carbon nitride/ferric oxide (GCN x /FO) photocatalysts were obtained by a one-step calcination method. The number of nitrogen defects was tuned by the application of KOH, while the ferric oxide phase and magnetism was controlled by the usage of ferrous oxalate. Interconversion between the hematite (α) and maghemite (γ) phases of Fe 2 O 3 was analyzed by X-ray diffraction, and magnetism of the GCN x -0.1/FO products provided via vibrating sample magnetometer test. The introduction of nitrogen defects narrowed the bandgap and extended the spectral range of light absorption while improving the ability to capture and activate N 2 effectively. Surface defects were employed as active sites, and the ammonia generation concentration reached approximately 69.7 μmol/L/h by N 2 photofixation under visible light. Due to their ease of synthesis and tuning, high photocatalytic activity, convenient and rapid collection for reuse, and excellent stability, GCN x /FO composited photocatalysts possess vast potential for use in clean ammonia production.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Zhengxiang Gu,Yijing Chen,Zengxi Wei,Linping Qian,Abdullah M. Al-Enizi,Jianmin Ma,Gang Zhou,Gengfeng Zheng
The electrochemical dinitrogen reduction represents an attractive approach of converting N 2 and water into ammonia, while the rational design of catalytic active centers remains challenging. Investigating model molecular catalysts with well-tuned catalytic sites should help to develop a clear structure-activity relationship for electrochemical N 2 reduction. Herein, we designed several polycyclic aromatic hydrocarbon (PAH) molecules with well-defined positions of boron and nitrogen atoms. Theoretical calculations revealed that the boron atoms possess high local positive charge densities as Lewis acid sites, which are beneficial for N 2 adsorption and activation, thus serving as major catalytic active sites for N 2 electrochemical reduction . Furthermore, the close vicinity of two boron atoms can further enhance the local positive density and subsequent catalytic activity. Using the PAH molecule with two boron atoms separated by two carbon atoms (B-2C-B), a high NH 3 production rate of 34.58 μg·h −1 ·cm −2 and a corresponding Faradaic efficiency (5.86%) were achieved at −0.7 V versus reversible hydrogen electrode, substantially exceeding the other PAHs with single boron or nitrogen-containing molecular structures.
研究领域:
化学
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材料科学
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电化学
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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
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2021
·
IF 6.901
Chaoqun Ma,Naihua Zhai,Bingping Liu,Shihai Yan
Although the electrochemical N 2 reduction reaction (NRR) to NH 3 provides a promising avenue for artificial N 2 fixation, building of efficient NRR electrocatalysts with high activity and stability remains a tremendous challenge. The combined experimental results and theoretical calculation reveal that MoS 2 with sulfur-vacancy defect (V S -MoS 2 ) is an admirable NRR catalyst. Electrochemical results demonstrate that V S -MoS 2 (5:2) possesses outstanding NRR performances, including a superior NH 3 average yield rate (46.1 × 10 −11 mol s −1 cm −2 at -0.5 V vs reversible hydrogen electrode (RHE)), an excellent faraday efficiency (FE: 4.58% at -0.4 V vs RHE), good electrochemical stability (at least 24 h), and high selectivity (no by-product of N 2 H 4 ). Density functional theory (DFT) calculations demonstrate that the rate determining steps (RDSs) of all V S -MoS 2 (010)-2, V S -MoS 2 (010)-1, and MoS 2 (010) are the first hydrogenation step to form *NNH intermediate, as reflected by the energy barriers of 0.06 eV, 0.20 eV, and 0.93 eV, the significantly charge transfer (1.02 e , 0.45 e vs. 0.41 e ) from two Mo atoms to N 2 , as well as the stretching of N N bond (1.200 Å, 1.140 Å vs. 0.970 Å), respectively. These results reveal that V S -MoS 2 (010)-2 can effectively activate inert N 2 molecule and have the potential application in nitrogen fixation under mild conditions.
研究领域:
材料科学
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电化学
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理论计算
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Renquan Guan,Dandan Wang,Yujun Zhang,Chen Liu,Wei Xu,Jiaou Wang,Zhao Zhao,Ming Feng,Qingkun Shang,Zaicheng Sun
Photocatalytic N 2 fixation (PNF) provides a low-cost route to generate ammonia. The poor conversion efficiency from photon to ammonia seriously hinders the step forward because of the low concentration of N 2 molecules. Herein, we demonstrate a photocatalyst with surface oxygen vacancies (Vo) and a F modified surface to facilitate N 2 adsorption and activation on the surface of catalysts. The Vo site promotes the chemical adsorption of N 2 , electron transfer from catalyst to N 2 . F modification switches the TiO 2 surface properties from hydrophilic to aerophilic, thus facilitating the adsorption of N 2 . Meanwhile, the hydrogen reduction reaction (HER) is suppressed, as protons hard to adsorb on F capped surfaces. The optimal NH 3 production rate can reach 206 μmolh −1 g −1 , which is ∼ 9 times higher than that of pure TiO 2 nanoparticles (∼23 μmolh −1 g −1 ). This report provides a potential strategy to overcome mass transfer limitation and achieve a high conversion efficiency in PNF.
研究领域:
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
Molecular Catalysis
·
2024
·
IF 3.9
Jingjing Wang,Zhiwei Liu,Liying Wang,Lu Li,Qian Liu,Zhiwei Liu,Zhenzhu Cao,Yongfeng Zhang,Lin Cheng,Jucai Yang
Combining pollutant degradation with nitrogen fixation has great potential for converting wastewater into suitable irrigation water. This approach purifies water by removing pollutants and provides essential nitrogen fertilizer nutrients to crops. In our investigation, we have introduced a new composite photocatalyst made by ligand anchoring Bi source of Bi 2 MoO 6 to reform BiMOF on the surface of sea-urchin-like Bi 2 MoO 6 spheres through the use of a solvothermal method. The 3D sea urchin spheres containing Bi 2 MoO 6 @BiMOF possess a large specific surface area and close-knit interfacial contacts, enabling ample channels for carrier migration. The composite has displayed impressive proficiency in breaking down pollutants and ammonia production. The elaborate, multi-channel structure within Bi-MOF enabled efficient N 2 or organic molecule adsorption, and Bi 2 MoO 6 generated plentiful photocarriers in reaction to visible light. The diverse interface between Bi 2 MoO 6 and BiMOF guaranteed successful photocarrier separation. The addition of methylene solution increased the yield of nitrogen fixation to 3080 (μmol/L/h/g), which is 15 times higher than that achieved in pure water. As the old saying goes, ``Falling red is not an unfeeling thing, it turns into spring mud and protects the flowers even more'', here although the addition of N 2 leads to a decrease in the degradation efficiency of methylene blue (MB), the addition of methylene blue (MB) consumes more holes and thus generates more photogenerated electrons, which greatly contributes to the production of NH 4 + and thus its application in agriculture. Additionally, These valuable insights highlight the possibility of transforming contaminated water into nutrient-rich, clean irrigation water for agricultural sustainability.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Longcheng Zhang,Qiang Zhou,Jie Liang,Luchao Yue,Tingshuai Li,Yongsong Luo,Qian Liu,Na Li,Bo Tang,Feng Gong,Xiaodong Guo,Xuping Sun
Electrochemical reduction of NO to NH3 is of great significance for mitigating the accumulation of nitrogen oxides and producing valuable NH3. Here, we demonstrate that the CoS nanosheet with sulfur vacancies (CoS1–x) behaves as an efficient catalyst toward electrochemical NO-to-NH3 conversion. In 0.2 M Na2SO4 electrolyte, such CoS1–x displays a large NH3 yield rate (44.67 μmol cm–2 h–1) and a high Faradaic efficiency (53.62%) at −0.4 V versus the reversible hydrogen electrode, outperforming the CoS counterpart (27.02 μmol cm–2 h–1; 36.68%). Moreover, the Zn–NO battery with CoS1–x shows excellent performance with a power density of 2.06 mW cm–2 and a large NH3 yield rate of 1492.41 μg h–1 mgcat.–1. Density functional theory was performed to obtain mechanistic insights into the NO reduction over CoS1–x.
研究领域:
材料科学
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电化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Small Methods
·
2019
·Vol. 3
·期 11
·1900356
·
IF 0
Tongwei Wu,Wenhan Kong,Ya Zhang,Zhe Xing,Jinxiu Zhao,Ting Wang,Xifeng Shi,Yonglan Luo,Xuping Sun
As a sustainable alternative technology to the Haber–Bosch process, electrochemical N 2 reduction offers the hope of directly converting N 2 to NH 3 at ambient conditions. However, its efficiency greatly depends on screening high-active electrocatalysts for the N 2 reduction reaction (NRR). Here, the recent experimental finding that V is an effective dopant to greatly improve the NRR performances of TiO 2 toward ambient N 2 -to-NH 3 fixation with excellent selectivity is reported. In 0.5 m anhydrous lithium perchlorate, V-doped TiO 2 nanorods attain a high Faradic efficiency of 15.3% and a large NH 3 yield of 17.73 µg h −1 mg cat. −1 at −0.40 and −0.50 V versus reversible hydrogen electrode, respectively, rivaling the performances of most reported aqueous-based NRR electrocatalysts. Density function theory (DFT) calculations are performed to gain further insight into the catalytic mechanism.
研究领域:
材料科学
·
化学工程
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理论计算
✓ 已验证
DOI
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