ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Jiangzhou Qin,Baojun Liu,Kwok-Ho Lam,Shijie Song,Xinyong Li,Xia Hu
To improve the photocatalytic efficiency of the N2 reduction reaction, MXene quantum dots (Ti3C2-QDs) and two-dimensional (2D) nickel metal–organic framework (Ni-MOF) with different ratios were fabricated by a simple self-assembly strategy to form type II heterojunctions. The resultant composites showed enhanced absorption and excellent interfacial charge-transfer capabilities according to the optical and photoelectron properties. The optimal Ti3C2-QD/Ni-MOF heterostructure exhibited a considerable ammonia yield rate (88.79 μmol gcat–1 h–1). By means of X-ray absorption near-edge fine structure (XANES) technique, it was found that the interaction of Ti3C2-QD and Ni-MOF could accelerate the electron transfer, and Ni site would be the main area to enrich the electron density as well as adsorb and activate N2. Finally, with the aid of density functional theory (DFT) calculations and in situ Fourier transform infrared spectrometry (FTIR), the reaction pathway and intermediate products were studied.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Ze Gao,Renming Liu,Daming Yang,Hongji Xu,Yuqi Wang,Bowen Li,Ming Feng,Ting Wang,Gangyong Jin
The adsorption and activation of N 2 as well as the competitive hydrogen evolution reaction (HER) pose significant challenges to the electrocatalytic nitrogen reduction reaction (ENRR), which severely limits its industrial application. Therefore, exploring the ENRR electrocatalysts with high activity and selectivity is an extremely important task. In this work, the oxygen vacancy-rich Fe 2 O 3 /Co 3 O 4 heterostructures (referred to as Vo-X-Fe 2 O 3 /Co 3 O 4 ) were rationally designed by employing Co 3 O 4 as a template via a simple hydrothermal and subsequent calcination method, which acted as highly efficient ENRR electrocatalysts. The electrocatalytic activity of Vo-X-Fe 2 O 3 /Co 3 O 4 can be easily regulated by optimization of the Fe content and the introduction of oxygen vacancy (Vo). The results demonstrate that the optimized Vo-1.0-Fe 2 O 3 /Co 3 O 4 catalyst achieves a high NH 3 yield of 47.37 μg h −1 mg cat −1 and a Faradaic efficiency (FE) of 22.42 %. Moreover, the excellent stability and reproducibility are also demonstrated. The comprehensive characterizations reveal that the exceptional performance of Vo-1.0-Fe 2 O 3 /Co 3 O 4 can be attributed to the improved N 2 adsorption and activation, restricted competitive HER and promoted electron transfer kinetics induced by the synergistic introduction of Vo and Fe. This work emerged a new speculating orientation for rational design of ENRR catalysts.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
Inorganic Chemistry Frontiers
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2022
·Vol. 10
·期 3
·869-879
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IF 7.779
Senda Su,Xiaoman Li,Mengyao Tan,Xu Zhang,Yingying Wang,Yanzhong Duan,Juan Peng,Min Luo
Layered double hydroxides (LDHs) have been shown to be efficient photocatalysts for the nitrogen fixation reaction. However, the effect of interlayer anions on the catalytic performance has not yet been reported. Herein, the anion regulated channel of LDHs blocked by carbonate (Car) was opened by controlling the suberate (Sub) intercalation, thus obtaining a series of ZnAl-LDHs with different anions (carbonate, suberate, PMo12−XVX, X = 0, 1, 2, 3, 8). The photocatalytic performance test in pure water showed that Sub@ZnAl-LDH and PMo9V3@ZnAl-LDH improved the NH3 yield from 11.37 μmol h−1 g−1cat for Car@ZnAl-LDH to 48.91 μmol h−1 g−1cat and 89.16 μmol h−1 g−1cat, respectively. The improvement of the performance was attributed to the following: (1) nitrogen was allowed to enter between LDH layers due to the expansion of the interlayer spacing; (2) the hydrophobic suberic acid intercalation suppressed the hydrogen evolution reaction; (3) the POM intercalation broadened the light absorption range of LDH. In this paper, the photocatalytic properties of ZnAl-LDHs intercalated with different anions are explored and investigated for the first time, which provides a versatile strategy for enhancing the catalytic activity of LDHs in the photocatalytic nitrogen fixation reaction.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xiaoyue Chen,Songge Zhang,Xiu Qian,Zhangqian Liang,Yanjun Xue,Xiaoli Zhang,Jian Tian,Ye Han,Minhua Shao
Herein, we assemble semi-metallic 1T′ phase MoS 2 on the surface Ti 3 C 2 MXene (1T′-MoS 2 /Ti 3 C 2 composite) by one-step hydrothermal method for nitrogen fixation. 1T′-MoS 2 /Ti 3 C 2 composites present a high ammonia yield rate of 31.96 µg h −1 mg −1 cat. at − 0.95 V vs. RHE and a Faradaic efficiency (FE) of 30.75% at − 0.7 V, which is much better than pure 1T′-MoS 2 and pure Ti 3 C 2 MXenes alone. Furthermore, the 1T′-MoS 2 /Ti 3 C 2 composites exhibit good selectivity and stability with no significant decrease in ammonia yield rate and FE. Density functional theory (DFT) calculations reveal that 1T′-MoS 2 /Ti 3 C 2 composite makes the activation and further reduction of *N 2 more thermodynamically favorable than pure 1T′-MoS 2 . 1 5 N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N 2 in the electrolyte.
研究领域:
材料科学
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电催化
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理论计算
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Yuyao Sun,Yi Han,Xinyi Zhang,Wenwen Cai,Yanyun Zhang,Yan Zhang,Zhenjiang Li,Bin Li,Jianping Lai,Lei Wang
Titanium dioxide (TiO 2 ) is widely used as a representative transition metal oxides (TMOs) catalyst for electrocatalytic nitrogen reduction reaction (NRR). However, the low stability, low selectivity, low ammonia (NH 3 ) yield and high overpotential of TiO 2 towards NRR strongly restricted its application in NRR. Here, we firstly add H to the lattice to synthesize a black TiO 2−x with oxygen vacancies (OVs) (B-TiO 1.8 ) for electrocatalytic NRR. After we optimized the amount of H and OVs, the NH 3 yield and stability can achieve 31.6 μg h −1 mg cat −1 and 100 h at − 0.1 V ( vs . RHE), respectively, the faradaic efficiency (FE) can achieve 47.7% at 0 V ( vs . RHE). In situ FTIR / ESR / XPS / TPD illustrate that OVs can promote the adsorption and activation of nitrogen (N 2 ), and lattice H can increase the number of OVs and stabilize them, suppress the hydrogen evolution reaction (HER) and promote the hydrogenation of N 2 .
研究领域:
材料科学
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电催化
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Ziyuan Xiu,Feng Wei,Xin Zhou,Xiaojun Han
Achieving high ammonia yield and Faraday efficiency is a long-sought-after goal in electrochemical N 2 fixation. Yet, the competitive hydrogen evolution in nitrogen reduction process and the low local concentration of nitrogen on the working electrode still limited the electrocatalytic performance. In the present contribution, a Fe-MoSe 2 nanosheet functioned with C18-thiol as a nano-hydrophobic surface was rationally constructed, which efficiently facilitated the three-phase contact of gas (N 2 ), liquid (H 2 O electrolyte), and solid (electrocatalyst). The fabrication of modified hydrophobic surface not only overcame the mass transfer limitation of N 2 and increased the local concentration of N 2 molecules on the catalyst, but also reduced the proton contact with electrocatalyst to inhibit HER. The three-phase electrocatalytic system achieved a high NH 3 yield of 34.75 μg h −1 mg −1 and outstanding Faraday efficiency of 23.31%. The adsorption and activation processes during NRR process were systematically investigated by the combination of experimental results and density function theory (DFT) simulations.
研究领域:
材料科学
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电化学
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催化反应
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DOI
高影响因子
ChemElectroChem
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2018
·Vol. 6
·期 4
·1014-1018
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IF 4.446
Rong Zhang,Haoran Guo,Li Yang,Yuan Wang,Zhiguo Niu,Hong Huang,Hongyu Chen,Li Xia,Tingshuai Li,Xifeng Shi,Xuping Sun,Baihai Li,Qian Liu
Graphical Hollow VO 2 microspheres can operate efficiently and stably to give an NH 3 yield of 14.85 μg h −1 mg −1 cat and a Faradaic efficiency of 3.97 % at −0.7 V (vs. the reversible hydrogen electrode) in 0.1 M Na 2 SO 4 , rivaling the performances of most reported aqueous-based electrocatalysts. Density functional theory calculations provide further insight into the catalytic mechanism involved. Electrochemical N 2 fixation has gained much attention as an environmentally friendly and sustainable process for NH 3 production at ambient conditions. Its efficiency depends greatly on identifying highly active electrocatalysts with good stability. In this work, we propose the use of VO 2 hollow microspheres as a robust non-precious metal catalyst for the N 2 reduction reaction (NRR). The catalyst operates efficiently and stably at neutral pH to high Faradaic efficiency (3.97 %) and NH 3 yield (14.85 μg h −1 mg −1 cat. ) under an applied potential of −0.7 V (vs. the reversible hydrogen electrode). Note that this catalyst also presents a high selectivity for NH 3 synthesis without N 2 H 4 generation. Density functional theory reveals that the energetically favorable pathway for NRR is *N 2 →*NNH→*NHNH→*NHNH 2 →*NH 2 NH 2 →*NH 2 +NH 3 →*NH 3 +NH 3 →2NH 3 , where the first hydrogenation step to form *NNH is the potential-determining step.
研究领域:
电催化
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材料科学
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理论计算
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Qun Ding,Xuejun Zou,Jun Ke,Yuying Dong,Yubo Cui,Hongchao Ma
Herein, a ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 heterojunction is successfully constructed through a facile hydrothermal strategy for enhancing solar energy harvesting and efficiency of catalytic nitrogen reduction induced by enlarged light absorption range, increasing interfacial charge transfer ability and desirable stability. Under the simulated sunlight irradiation, the N 2 fixation experiment shows that the yield of NH 3 reaches 1084.31 μmol/(g·h) over the TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalyst, and the yield is significantly enhanced, which is 33.68 and 13.94 times that is higher than the pure TiO 2 and g-C 3 N 4 , respectively. In a mean time, the excellent performance of the photocatalytic N 2 fixation over the ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is verified based on density function theory calculation and the decisive step over the composite is investigated by calculating Gibbs free energies of nitrogen reduction paths. The performance enhancement mechanism of TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is speculated, which indicates that the hybridized three-component system presents a desirable Z-scheme band alignment, resulting in the improvement of separation and transfer efficiency of photoinduced charge carriers. The article shows a new and high-efficiency TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalysis for excellent nitrogen reduction ability.
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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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
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2019
·Vol. 7
·期 20
·12526-12531
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IF 10.733
Hongjie Yu,Ziqiang Wang,Dandan Yang,Xiaoqian Qian,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
The electrochemical nitrogen reduction reaction (NRR) is considered as a facile and sustainable strategy for ammonia production. Design of high-performance electrocatalysts is the crucial issue for the NRR. Herein, we present a one-pot reduction method to directly synthesize bimetallic Ag3Cu porous networks (Ag3Cu BPNs). Owing to their porous networks and bimetallic composition, the Ag3Cu BPNs exhibit outstanding NRR performance with a high NH3 yield of 24.59 μg h−1 mgcat.−1 and faradaic efficiency of 13.28% at −0.5 V vs. the reversible hydrogen electrode. This study proposes a facile and scalable route for the development of metallic porous networks with an interconnected structure and desired components for electrochemical ammonia production.
研究领域:
电化学
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材料科学
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催化
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可持续化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Hao Ying,Tingting Chen,Chenyun Zhang,Jiahui Bi,Zhonghao Li,Jingcheng Hao
The production of ammonia through electrocatalytic nitrogen reduction reaction (NRR) is environmentally friendly and energy-saving, but it still suffers from the low NH 3 yield rate and poor selectivity. Herein, enlightened by the unique solubility of Fe 3 O 4 in deep eutectic solvent (DES), we, for the first time, reported a DES-based regeneration strategy to fabricate porous Fe 3 O 4 nanosheets utilizing commercial Fe 3 O 4 powder as raw materials. The as-regenerated porous Fe 3 O 4 nanosheets exhibited satisfactory electrocatalytic performance toward NRR, affording a NH 3 yield rate of 12.09 μg h −1 mg −1 cat along with an outstanding Faradaic efficiency (FE) of 34.38% at −0.1 V versus reversible hydrogen electrode (RHE), in the 0.1 M Na 2 SO 4 electrolyte. The superior electrocatalytic activity of the as-regenerated Fe 3 O 4 nanosheets mainly resulted from their unique sheet-like morphology with large active surface area, high porosity, and abundant oxygen vacancies. Our proposed DES-based regeneration strategy opens a new avenue for the construction of high-performance electrocatalyst from commercial raw materials, holding great promise in NRR.
研究领域:
材料科学
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环境科学
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2019
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IF 3.261
Yuan Liao,Jiannan Lin,Baihua Cui,Gang Xie,Shi Hu
Photocatalytic nitrogen fixation has been burgeoning since the 20th century because the conventional Haber–Bosch process is quite energy-intensive, so other sustainable alternatives are highly required. This work uses a facile way to synthesize ultrasmall metal ruthenium on TiO 2 (P25) for photocatalytic nitrogen fixation at ambient temperature and pressure. The metal ruthenium is 2–3 nm in size and evenly dispersed over TiO 2 (P25). Both Indophenol method and ion chromatography are used to detect the ammonia yield, and possible mechanism is also proposed.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 18
·8920-8926
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IF 11.301
Ying Liu,Xiaorong Zhu,Qinghua Zhang,Tang Tang,Yun Zhang,Lin Gu,Yafei Li,Jianchun Bao,Zhihui Dai,Jin-Song Hu
The development of efficient and cost-effective electrocatalysts is essential for the electrochemical reduction of N2 to produce NH3 under ambient conditions. Herein, various well-dispersed Mo-based nanoparticles are selectively synthesized to reveal the influences of the compositions and hetero-interfaces on the performance for the N2 reduction reaction (NRR). Systematic experiments discovered that compared with single-component Mo2C or Mo nanoparticles, the heterostructured binary MoC/Mo2C and ternary Mo/MoC/Mo2C nanoparticles exhibit significantly enhanced NRR performance by creating abundant hetero-interfaces. Moreover, theoretical calculations reveal that the integration of metallic Mo with MoC/Mo2C appreciably reduces the energy demand for NH3 desorption, contributing to the enhanced NRR process. As a result, a remarkable NH3 yield rate of up to 20.4 μg h−1 mg−1 and a FE up to 18.9% can be achieved. These findings suggest that engineering crystalline phases and hetero-interfaces represents a new avenue for advancing the electrocatalytic performance of a NRR catalyst.
研究领域:
材料科学
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电化学
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催化
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产品关联
DOI
高影响因子
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