Chem
·
2024
·
IF 19.1
Xiaoran Zhang,Xiaorong Zhu,Shuowen Bo,Chen Chen,Qingfeng Zhai,Shuang Li,Xiaojin Tu,Jianyun Zheng,Dongdong Wang,Xiaoxiao Wei,Wei Chen,Tehua Wang,Yafei Li,Qinghua Liu,San Ping Jiang,Liming Dai,Shuangyin Wang
Electrocatalysis offers a sustainable approach to artificial nitrogen fixation yet faces numerous challenges. Selective synthesis of nitrogen-containing compounds shows promise but needs significant improvement. Herein, we demonstrate selective ammonia and urea synthesis via co-electrolysis with CO 2 . High CO binding energy on Re-Mn catalysts leads to the formation of ∗C species, which serve as electron reservoirs to enhance N 2 activation for C-N coupling (N 2 + ∗C → ∗CN 2 ), followed by C-N dissociation. This results in ammonia production with a yield rate of 48.9 ± 2.4 mg g −1 h −1 and an N-selectivity of 98.4%. In contrast, Zn-Mn sites, characterized by low CO binding, facilitate the migration of CO and its coupling with adsorbed N 2 (CO + ∗N=N∗ → ∗NCON∗). Subsequent hydrogenations of ∗NCON∗ promote urea synthesis with an N-selectivity of 89.1%. Utilizing Janus coupling with two C-N pathways aims to meet energy, agriculture, and chemical industry demands. We realized the selective synthesis of ammonia and urea, respectively, in one electrocatalytic system for the first time by Janus coupling with two distinguishable C-N coupling paths from N 2 and CO 2 .
研究领域:
化学工程
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能源科学
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农业科学
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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
JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Zhipeng Zhang,Feifei Li,Guoqiang Li,Rui Li,Yunfang Wang,Yawen Wang,Xiaochao Zhang,Lulu Zhang,Fangfang Li,Jianxin Liu,Caimei Fan
The bottlenecks of photocatalytic nitrogen fixation are adsorption and activation of nitrogen, because N–N bond in dinitrogen is one of the strongest bonds in chemistry . Herein, for the first time, Cu-doped MIL-101(Fe) was applications in photocatalytic nitrogen fixation. The photocatalytic nitrogen fixation activity of Cu-MIL-101(Fe) is three times that of MIL-101(Fe). Characteristic of MIL-101(Fe) and Cu-MIL-101(Fe) are systematically compared by XRD , SEM, TEM, BET, PL and energy band structure . These results indicated that the Cu doping not only enlarge the specific surface area from 1413 m 2 /g to 2097 m 2 /g, but also increase the photoreduction capability from −0.13 V to −0.7 V. These results indicated that nitrogen adsorption and activation capacity can be improved by Cu doping. By combining metal ions doping and components regulation of MOFs , this work provides many future opportunities for enhance photocatalytic nitrogen fixation activity.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 32
·17442-17450
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IF 12.732
Yintong Zhang,Feng Du,Ruyi Wang,Xintong Ling,Xiaoyong Wang,Qing Shen,Yujie Xiong,Tao Li,Yong Zhou,Zhigang Zou
The electrocatalytic nitrogen oxidation reaction (NOR) is a promising alternative to the industrial synthesis of nitrate. However, with the enhancement of NOR activity by modification methods, the competitive oxygen evolution reaction (OER) is always improved simultaneously. Here, a hybrid electrocatalyst composed of Au nanoparticles and oxygen vacancy-enriched niobium oxide nanobelts (Au–Nb2O5−x) was prepared on niobium foil for N2 fixation into NO3−. The results of X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) demonstrate that electron transfer occurs between Au nanoparticles and the oxygen vacancies in Nb2O5−x nanobelts, which adjusts the electronic structures of oxygen vacancies near the Au/Nb2O5−x interface. Electrochemical and N2 temperature-programmed desorption (TPD) tests indicate that the optimization of the electronic structure suppresses the activity of the competitive OER on oxygen vacancy sites and facilitates nitrogen adsorption on the surface of Au–Nb2O5−x, which significantly enhances the NOR performance of the electrocatalyst.
研究领域:
电化学
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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
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Zhenyu Liu,Xiaoman Li,Senda Su,Wenming Ding,Linghu Meng,Yingying Wang,Mengyao Tan,Min Luo
Energy band engineering strategy by doping has been extensively proved to have great influence on photocatalytic properties of semiconductors. Herein, a novel Co-doped Bi 2 MoO 6 (Co-BMO) photocatalyst was developed for photocatalytic nitrogen fixation. Co-BMO with microsphere structure was synthesized by a one-step solvothermal method. The NH 3 yield of 0.3 % Co-BMO (130.07 μmol·h −1 ·g cat −1 ) was about 3.9 times higher than that of pure BMO without scavengers and visible light irradiation. The band gap of 0.3 % Co-BMO was reduced and the average PL lifetime was improved due to the successful doping of Co 2+ , which directly led to higher separation efficiency of photogenerated carriers and improved photocatalyst activity. In addition, gas chromatography (GC) tests showed that 0.3 % Co-BMO had a higher photocatalytic oxygen production capacity, which meant that more protons would be involved in the nitrogen reduction reaction . Their synergistic effect greatly enhanced the photocatalytic nitrogen fixation ability of 0.3 % Co-BMO. This novel photocatalyst may be a promising candidate for photocatalytic nitrogen fixation.
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
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Can Sun,Runze Guo,Zhexiao Zhu,Shouxin Zhu,Jingyi Qu,Zijie Fang,Xiaolu Xu,Jiahui Lin,Yangben Chen,Shijie Zhang,Hui Zheng
Photocatalytic nitrogen fixation as a green, environmentally friendly, mild and low energy-consuming nitrogen fixation is considered as an ideal way to produce ammonia. Herein, inspired by nitrogen-fixing enzymes, the MOF materials Fe-sdc and Ti-sdc were synthesized by a simple solvothermal synthesis method using Fe and Ti as metal nodes and 4,4′-stilbenedicarboxylic acid (H 2 sdc) as a ligand. The ammonia production rates of Fe-sdc and Ti-sdc were 61.01 μmol g −1 h −1 and 46.84 μmol g −1 h −1 . The 15 N 2 isotope experiments were utilized to determine the nitrogen source for ammonia synthesis during the nitrogen fixation process of Fe-sdc. Various characterization analyses were also utilized to analyze the reasons for the better nitrogen fixation performance of the two catalysts.
研究领域:
材料科学
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环境科学
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催化化学
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Yuanhang Feng,Zhao zhao,Ting Wang,Jiaming Li,Ming Xu,Hailiang Jiao,Chen Wang,Haibo Li,Ming Feng
Photocatalytic N 2 fixation is a promising and sustainable manufacturing process of ammonia (NH 3 ); however, the NH 3 production rate by this method is very low, thus severely restricting further application of this sustainable technology. Therefore, developing an efficient photocatalyst for N 2 fixation under mild conditions is urgently required. Herein, ferroelectric Bi 2 WO 6 materials with different surface oxygen defects were prepared, and the concentration of corresponding defects was controlled by adjusting the thermal reduction time. The abundant oxygen defects in Bi 2 WO 6 can provide more reactive sites to promote the effective adsorption of N 2 , and the photogenerated charge carrier can be efficiently separated benefiting from the internal electric field. These would weaken the N 2 triple bond and reduce the activation energy barrier for the conversion of N 2 to NH 3 under mild conditions. In the absence of sacrificial agents and cocatalysts, the optimized Bi 2 WO 6 with oxygen defects shows an indigenous NH 3 yield of 132.175 μmol·g -1 ·L -1 ·h -1 , which is more than two times higher than that of the original Bi 2 WO 6 . Surprisingly, the Bi 2 WO 6 with oxygen defects produced more than eight times NH 3 (471.13 μmol·g -1 ·L -1 ·h -1 ) than that of the original Bi 2 WO 6 when assisted by an external magnetic field, thus providing a new perspective for further enhancing the N 2 fixation performance.
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
CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Junyu Fan,Meimei Zuo,Zhaoxia Ding,Zhiwei Zhao,Jie Liu,Bo Sun
A promising and practicable catalyst is the key challenge for industrial perspective to promote photocatalytic nitrogen fixation. In this study, a new 0D /2D heterojunction, oxygen vacancy-induced In(OH) 3 /carbon nitride (OV-In(OH) 3 /CN), was synthesized by generating In(OH) 3 nanoparticles on g-C 3 N 4 nanosheets in the presence of glyoxal through a facile and readily precipitation growth method at 60℃and under atmospheric pressure. The existence of oxygen vacancies, structure, morphology and optical-electronic properties of the composite were characterized by HRTEM, XPS and EPR analysis and other measurements. The OV-In(OH) 3 /CN heterojunction exhibited excellent photocatalytic activity for nitrogen fixation with a good chemical stability. The OV-In/CN-3 sample reached the maximum NH 3 generation rate to be 3.81 mM*h −1 *g −1 , which was about 10 times as that of pure g-C 3 N 4 and was also higher than that of other catalysts reported. Though the In(OH) 3 in heterojunction was demonstrated incapable of producing photogenerated electrons under vis-light irradiation, its oxygen vacancy was found to “receive” and “trap” some excited electrons from g-C 3 N 4 , promoting electron-hole pairs separation efficiency and prolonging the lifetime of carriers. And it also can introduce many chemisorption sites for N 2 . Those are the two key reasons for its high photocatalytic activity.
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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产品关联
DOI
高影响因子
Environmental Progress & Sustainable Energy
·
2023
·
IF 2.8
Ping Gao,Xinshan Rong,Shixian Zhang,Ting Sun,Jun Liu,Xuchun Qiu,Xiangtong Zhou,Zhiren Wu,Jing Wei
Solar-driven reduction of nitrogen to ammonia is a promising green approach and is considered as a sustainable alternative to the Haber–Bosch process. Carbon nitride (g-C 3 N 4 ) is an ideal non-metallic semiconductor photocatalyst for photocatalytic N 2 reduction reaction (p-NRR). In this work, we designed a simple supramolecular self-assembly method to prepare copper-doped porous graphitic nitride (Cu@pg-C 3 N 4 ) photocatalysts. The synergistic semiconductor and metal interactions enabled the obtained Cu@pg-C 3 N 4 to achieve larger specific surface area, more efficient photogenerated carrier separation, and stronger photoreduction ability. The specific surface area of Cu@pg-C 3 N 4 increased from 5.69 to 75.76 μmol/L, exposing more active sites compared to bulk g-C 3 N 4 . The NH 4 + production rate of the obtained Cu@pg-C 3 N 4 was 150.47 μmol/L, which is 20 times higher than that of the bulk carbon nitride, exhibiting excellent N 2 photofixation ability. These findings highlight the significant progress that can be achieved by metal supramolecular network modification strategies in harnessing the potential of carbon nitride for photocatalytic reduction applications.
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
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jianli Chen,Shuoshuo Zang,Kaiyue Gao,Chengming Zhang,Xiufang Wang,Hewen Liu
Herein, a novel ultrathin 2D/2D heterostructure, Bi 12 O 17 Br 2 with oxygen vacancies/ZnCr layered double hydroxides (V o -Bi 12 O 17 Br 2 /ZnCr-LDHs, V o -BZ) is prepared by solvothermal and coprecipitation methods for photocatalytic reduction of N 2 to NH 3 . The optimal 2D/2D V o -BZ heterostructure photocatalyst shows production rate of ammonia production of 286.0 μmol·g −1 ·h −1 . It is 12.5 and 3.6 times higher than that of pure ZnCr-LDHs and V o -Bi 12 O 17 Br 2 . The improved photocatalytic nitrogen reduction performance is attributed to the intimate contact interface, matching bandgap structure, the shortened migration distance, and thus significantly improved separation and transfer efficiency of hole-electron pairs and light adsorption ability. The large number of oxygen vacancies and high specific surface promote the absorption, activation and deionization of N 2 molecules. The theoretical simulation calculation indicates that the free energy of nitrogen molecules on the surface of Vo-BZ is favorable for the absorption and activation of N 2 molecules. The existence of oxygen vacancies and formation of heterojunctions can dramatically reduce energy barrier of nitrogen molecule hydrogenation process to boost photocatalytic N 2 reduction. This study provides a new idea for the development of efficient photocatalytic nitrogen fixing catalysts.
研究领域:
材料科学
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环境科学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Bowen Chen,Yuanwen Hou,Hanke Li,Hejun Gao,Hongquan Fu,Fang Liao,Juan Zhang,Yunwen Liao
The catalytic conversion of nitrogen to ammonia is one of the most significant processes in nature and the chemical industry. However, the traditional Haber-Bosch process of ammonia synthesis consumes substantial energy and emits a large amount of carbon dioxide . The efficiency of photocatalytic N 2 activation is severely limited by the lack of N 2 adsorption sites and poor carrier utilization. Herein, an efficient α-Bi 2 O 3 /Bi 3 O 4 Br heterojunction is proposed with a photocatalytic nitrogen fixation activity of 238.67 μmol·g −1 ·h −1 . Compared with the BiOBr precursor, α-Bi 2 O 3 and Bi 3 O 4 Br, the α-Bi 2 O 3 /Bi 3 O 4 Br heterojunction with oxygen vacancies can improve the adsorption and activation capacity of N 2 and promote the separation efficiency of charge carrier pairs by accommodating photogenerated electrons under visible light through the mechanism of N -type semiconductors. Therefore, oxygen vacancies and heterojunction engineering of semiconductive nanomaterials provide a promising method for the rational design of photocatalysts to enhance the rate of ammonia synthesis under mild conditions.
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
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 34
·13085-13093
·
IF 4.569
Lijun Guo,Feifei Li,Jianxin Liu,Zehui Jia,Rui Li,Zhuobin Yu,Yawen Wang,Caimei Fan
The scaling relations between nitrogen adsorption and NHx destabilization are key challenges to the widespread adoption of the photocatalytic synthesis of ammonia. In this work, a FeII-rich MIL-101(Fe) (MIL-101(FeII/FeIII)) was synthesized using a one-step solvent thermal method with ethylene glycol (EG) as a reducing agent, which can break the scaling relationship by photoinduced FeII (high nitrogen adsorption ability) and FeIII (high NHz destabilization ability) cycling. XPS was used to detect the change in iron valence state in the MIL-101(FeII/FeIII) material. The photocatalytic nitrogen fixation efficiency of MIL-101(FeII/FeIII) under visible light without any sacrificial agent was 466.8 μmol h−1 g−1, five times that of MIL-101(Fe). After photocatalytic experiments, MIL-101(FeII/FeIII) retained an unchanged FeII/FeIII rate, indicating that this FeII/FeIII cycling can be maintained. DFT modeling of the FeII-rich MOF material showed that a FeII1 FeIII2 system has a higher N2 activation capacity than a FeIII3 system. The catalytic mechanism was further proved by in situ infrared spectra and N15 isotopic tracers. Therefore, the improvement of photocatalytic activity was mainly attributed to the change in the nitrogen adsorption capacity during the photoinduced FeII/FeIII cycling.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
DOI
高影响因子
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