Nature Communications
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2025
·Vol. 16
·期 1
·1-10
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IF 15.7
Yang Wenqiang,Liu Huan,Chang Xiaoxia,Zhang Yunlong,Cai Yafeng,Li Yifan,Cui Yi,Xu Bingjun,Yu Liang,Cui Xiaoju,Deng Dehui
Electrocatalytic NO reduction reaction (NORR) offers a promising route for sustainable NH 3 synthesis along with removal of NO pollutant. However, it remains a great challenge to accomplish both high NH 3 production rate and long duration to satisfy industrial application demands. Here, we report an in situ-formed hierarchical porous Cu nanowire array monolithic electrode ensembled in a pressurized electrolyzer to regulate NORR reaction kinetics and thermodynamics, which delivers an industrial-level NH 3 partial current density of 1007 mA cm –2 with Faradaic efficiency of 96.1% and remains stable at 1000 mA cm –2 for 100 hours. Integrating the Cu nanowire array monolithic electrode with pressurized electrolyzer boosts the NH 3 production rate to 10.5 mmol h –1 cm –2 , which is over tenfold that using commercial Cu foam at 1 atm. The NORR performance can be attributed to the promoted NO mass transfer to the enriched Cu surface, which could increase the NO coverage on Cu and then destabilize adsorbed NO and weaken hydrogen adsorption, thereby facilitating NO hydrogenation to NH 3 while suppressing the competing hydrogen evolution.
研究领域:
化学工程
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环境科学
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材料科学
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PubMed
高影响因子
Frontiers in Chemistry
·
2018
·
IF 4.155
Zhu Chonghui,Cheng Xiaoli,Dong Xin,Xu Ying ming
PANI/TiO2 nanocomposites spheres were synthesized using a simple and efficient one-step hydrothermal process. The morphology and structure of PANI/TiO2 nanocomposites spheres were investigated by X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques. The PANI/TiO2 nanocomposite sphere-based sensor exhibits good selectivity, sensitivity (5.4 to 100 ppm), repeatability, long-term stability and low detection limit (0.5 ppm) to ammonia at room temperature (20 ± 5°C). It also shows a good linearity relationship in the range of 0.5–5 and 5–100 ppm. The excellent NH3 sensing performance is mainly due to the formation of the p-n heterostructure in the nanocomposites.
研究领域:
材料科学
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化学传感器
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PubMed
高影响因子
Journal of Materials Research and Technology-JMR&T
·
2021
·
IF 5.039
Yongjie Liu,Ran Xin,Donglai Ma,Qingqing Hu,Yue Wang,Zhixiong You
Ferrovanadium nitride, which comprises V and N, is an important alloy additive for the production of high-strength low-alloy steel. As an efficient reducing agent and nitrogen source, ammonia gas is widely used in the preparation of metal nitrides. In this study, ferrovanadium nitride alloy powder is prepared by reducing and nitriding VO 2 /Fe 2 O 3 in NH 3 –H 2 gas mixtures with different nitriding potentials. Thermodynamic analysis indicate that the reduction and nitridation of VO 2 and Fe 2 O 3 is feasible. VO 2 is converted into VN, whereas Fe and Fe 4 N can be formed depend on the reaction conditions. Lower temperatures and higher nitriding potentials are beneficial to the formation of Fe 4 N. Based on Rietveld refinement analysis, the formation of Fe 4 N and the atomic occupancy of V and N in vanadium oxynitride, which is associated with the temperature, reaction time, and nitriding potential, is determined. A ferrovanadium nitride alloy powder with an O content of 0.26 wt.% is prepared by reducing and nitriding VO 2 /Fe 2 O 3 at 900 °C for 1 h at a nitriding potential of 4.4 × 10 −3 Pa −0.5 .
研究领域:
材料科学
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冶金工程
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DOI
高影响因子
Cell Reports Physical Science
·
2022
·
IF 7.832
Jaysree Pan,Qianru Wang,Jianping Guo,Heine Anton Hansen,Ping Chen,Tejs Vegge
Ammonia is a central vector in sustainable global growth, but the usage of fossil feedstocks and centralized Haber-Bosch synthesis conditions causes >1.4% of global anthropogenic CO 2 emissions. While nitrogenase enzymes convert atmospheric N 2 to ammonia at ambient conditions, even the most active manmade inorganic catalysts fail due to low activity and parasitic hydrogen evolution at low temperatures. Here, we show that the [RuH 6 ] catalytic center in ternary ruthenium complex hydrides (Li 4 RuH 6 ) activates N 2 preferentially and avoids hydrogen over-saturation at low temperatures and near ambient pressure by delicately balancing H 2 chemisorption and N 2 activation. The active [RuH 6 ] catalytic center is capable of achieving high yield at low temperatures via a shift in the rate-determining reaction intermediates and transition states, where the reaction orders in hydrogen and ammonia change dramatically. Temperature-dependent atomic-scale understanding of this unique mechanism is obtained with synchronized experimental and density functional theory investigations.
研究领域:
化学
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材料科学
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DOI
高影响因子
CATALYSIS TODAY
·
2019
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IF 4.888
Shuohan Yu,Yiyang Lu,Fei Gao,Lin Dong
In this work, TiO 2 nano-octahedron and nano-rods were successfully synthesized, and Cu oxides were loaded on them. Structures of CuO/TiO 2 catalysts were studied by XRD, TEM, and Raman techniques. It was founded that TiO 2 nano-octahedron and nano-rods dominantly exposed (101) and (100) facets of TiO 2 , respectively. Cu cations located in tetrahedral vacant sites on (101) facet of TiO 2 and coordinated with 4 neighbor oxygen, whereas it located in octahedral vacant sites on (100) facet of TiO 2 and coordinated with 6 neighbor oxygen, which resulted in redox cycle Cu 2+ +Ti 3+ ⟵→Cu + +Ti 4+ and more acid sites on surface of CuO/TiO 2 nano-octahedron, and thus the enhanced NH 3 -SCR performance.
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高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Zhenhua Liu,Tengfei Zhang,Shunlong Ju,Yanda Ji,Zhaotong Hu,Yingtong Lv,Guanglin Xia,Xuebin Yu
Lithium borohydride (LiBH4), with high compatibility to lithium anode, low grain boundary resistance, and light mass, is regarded as a promising solid-state electrolyte. However, poor ionic conductivity at room temperature limits its practical application in all-solid-state lithium-ion batteries (ASSLBs). In the present study, Li(NH3)xBH4@SiO2 (0 ≤ x ≤ 0.5) composites were obtained by ammonia absorption and simple ball-milling. Among them, Li(NH3)0.5BH4@SiO2 exhibits a high ionic conductivity of 3.95 × 10–2 S cm–1 at 60 °C, with a lithium transference number up to 0.9999 at 30 °C. More importantly, the experimental results and density functional theory (DFT) calculations show that the skeleton and interfacial interaction of silica can effectively improve the electrochemical performance of the full cell. All-solid-state lithium–sulfur batteries exhibit a specific discharge capacity of 1221.7 mAh g–1 after 10 cycles. Reversible capacities of 1589, 1381, 1176, 969, and 695 mAh g–1 could be achieved at 0.1, 0.2, 0.3, 0.5, and 1C, respectively. These findings prove that Li(NH3)xBH4@SiO2 is an attractive electrolyte for next-generation ASSLBs.
研究领域:
材料科学
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固体离子学
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储能
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电化学
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DOI
高影响因子
Advanced Science
·
2025
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IF 14.1
Chaomin Duan,Meng Wang,Yan Zhang,Zhihua Lian,Wenpo Shan
Ammonia (NH 3 ) emissions adversely affect both the environment and human health. The selective catalytic oxidation of NH 3 (NH 3 -SCO) holds great promise for NH 3 abatement; however, there remains a lack of cost-effective NH 3 -SCO catalysts with high activity and N 2 selectivity for practical applications. This study reports on a strategy for constructing an outstanding NH 3 oxidation catalyst via the in situ doping of Cu into CeO 2 nanorods. The designed CeCuO x nanorod catalyst shows remarkable activity, N 2 selectivity, and stability for NH 3 oxidation, achieving complete conversion below 250 °C, with ≈80% N 2 selectivity. The results of various characterization tests and density functional theory (DFT) calculations show that the addition of Cu induces the formation of abundant Cu + -O v -Ce 3+ active sites on the CeO 2 , which are beneficial for the adsorption and activation of reactants. Additionally, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) confirms that the addition of Cu switches the primary intermediate species of NH 3 oxidation from bidentate nitrate species to monodentate nitrate species, which accelerates the rate-determining step of NH 3 -to-N 2 oxidation. Therefore, doping Cu into CeO 2 greatly improves its NH 3 oxidation activity and N 2 selectivity. This study provides valuable insights into the construction of highly active sites for NH 3 oxidation.
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PubMed
高影响因子
Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 6
·2715-2723
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IF 6.482
Xiaojing Feng,Zhongnan Guo,Xiaoxiao Yan,Jun Deng,Dan Wu,Zijing Zhang,Fan Sun,Wenxia Yuan
Metal phosphorus trichalcogenides (MPX3) are of great interest since these layered materials exhibit wide applications in optical, electrical and magnetic fields. An effective chemical intercalation route for MPX3 which could regulate their physical properties, however, is still lacking. In this work, we show that the liquid ammonia method is an efficient route to co-intercalate alkali metals and NH3 molecules into the gaps in FePS3. After intercalation, the interlayer distance is significantly enlarged by ∼3 Å while the monoclinic lattice (C2/m space group) is still maintained. The structure refinement and EDS measurement suggest that intercalation does not induce any Fe vacancy, thus leading to electron transfer from the alkali metal to [FePS3] layers. Interestingly, magnetic susceptibility shows that the intrinsic anti-ferromagnetic transition in the FePS3 matrix is completely suppressed by this intercalation, whereas a spin-glass state is observed in A(NH3)xFePS3 (A = Li, K) in the lower temperature range (<50 K). The intercalation described in this work is reversible: the alkali metal can be easily de-intercalated using a two-step route and the anti-ferromagnetism reappears accordingly. Meanwhile, the liquid ammonia method is also shown to be efficient at intercalating other MPS3 materials (M = Mn, Co, Ni). Our work not only enriches the intercalation chemistry in the MPX3 system but also provides an excellent route to regulate the magnetic properties of these layered materials.
研究领域:
材料科学
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无机化学
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凝聚态物理
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纳米技术
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功能材料
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2022
·Vol. 33
·期 9
·6168-6177
·
IF 2.779
Chen Pu,Zhao Zhihua,Shao Zhigang,Tian Ye,Li Bo,Huang Bo,Zhang Shuaiwen,Liu Chunbo,Shen Xiaoqing
Semiconducting nanomaterials with different sizes and shapes have wide applications in the field of electronics, and one of the key pathway to improve their performance is by recombination of different materials. In our innovative work, the nanocomposites of polypyrrole (PPy) and MXene were prepared by a simple in situ polymerization reaction. The samples were characterized by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). The samples were made into sensors, and the gas sensitivities of the materials were investigated under different test conditions. The results showed that the response value of PPy/MXene-12 sensor to 100 ppm ammonia at room temperature was 2.38 times than that of pure PPy and 6.38 times than that of pure MXene. In addition, the sensor has excellent selectivity and low detection limit, which demonstrate the excellent practicability of them in the field of Internet of Things (IoT).
研究领域:
材料科学
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电子工程
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DOI
高影响因子
JOURNAL OF ELECTRONIC MATERIALS
·
2021
·Vol. 50
·期 11
·6414-6425
·
IF 1.938
Fan Wentao,Du Yongqiang,Zhou Jianjun,Ma Xueqing,Liu Yingliang,Xu Shengang,Cao Shaokui
The introduction of polymer additives provides a simple effective method to modify perovskite grain boundaries to improve power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs). In this work, the high-quality methylammonium lead triiodide (MAPbI 3 ) perovskite film is prepared by adding the protonated polyamide-amine dendrimer (NH 3 + -PAMAM) to the perovskite precursor solution to regulate the crystalline growth process. The cross-linked perovskite grain structure induced by dendritic NH 3 + -functionalized PAMAM macromolecules results in the formation of compact and pinhole-free perovskite film owing to the suppression of perovskite gain boundaries. Finally, the unsealed NH 3 + -PAMAM modified PSC device achieves the highest PCE value of 16.03%, representing an increase of 48% compared with the control PSC device. Also, the unencapsulated NH 3 + -PAMAM-modified PSC device retained 75% of initial PCE value after being exposed to an ambient environment for 20 days, which is obviously higher than 10% for the control device. The improvements of perovskite morphology and photovoltaic performance are attributed to the modification of NH 3 + -PAMAM dendrimers. Graphic abstract
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CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Li Li,Haijun Chen,Lei Li,Baihai Li,Qianbao Wu,Chunhua Cui,Biao Deng,Yonglan Luo,Qian Liu,Tingshuai Li,Fang Zhang,Abdullah M. Asiri,Zhe-Sheng Feng,Yan Wang,Xuping Sun
Electrochemical N 2 reduction provides a green and sustainable alternative to the Haber-Bosch technology for NH 3 synthesis. However, the extreme inertness of N 2 molecules is a formidable challenge, which requires the development of an active electrocatalyst to drive the N 2 reduction reaction (NRR) for NH 3 production at ambient conditions. Herein, we demonstrate the development of La-doped TiO 2 nanorods as an efficient NRR electrocatalyst for ambient NH 3 synthesis. The optimized La-TiO 2 catalyst offers a large NH 3 yield of 23.06 μg h −1 mg cat −1 and a high Faradaic efficiency of 14.54% at –0.70 V versus reversible hydrogen electrode in 0.1 M LiClO 4 , outperforming most La- and Ti-based catalysts reported before. Significantly, it also demonstrates high electrochemical stability and its activity decay is negligible after 48 h test. The mechanism is further revealed by density functional theory calculations.
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JOURNAL OF MOLECULAR LIQUIDS
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2020
·
IF 5.065
Lei Yuan,Hongshuai Gao,Haiyan Jiang,Shaojuan Zeng,Tao Li,Baozeng Ren,Xiangping Zhang
A novel type of dual-functionalized pyridinium-based ionic liquids (ILs) with acidic protons and hydroxyl groups , were designed and synthesized for ammonia (NH 3 ) absorption. The NH 3 absorption isotherms in dual-functionalized pyridinium-based ILs at temperatures from 303.15 to 343.15 K and pressures up to 600 kPa were computed using gas-liquid equilibrium method. It revealed that 4-pyridinemethanol bis(trifluoromethane)sulfonamide [4-MeOHPy][NTf 2 ] showed the maximum NH 3 solubility of 3.43 mol NH 3 /mol IL at 313.15 K and atmospheric pressure, surpassing any nonmetallic ILs previously reported. Furthermore, the characteristics of isotherms under low pressures behaved an obvious chemical reaction between ILs and NH 3 , and all experimental solubilities were regulated by a reaction equilibrium thermodynamic model (RETM). The thermodynamic properties were further obtained to better understand the NH 3 absorption process. The results indicated that this model endorses the 1:1 (NH 3 -IL) mole ratio of chemical reaction mechanism and the reaction enthalpy is main driving force of NH 3 absorption in ILs.
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