JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2021
·
IF 8.067
Tayiba Ilyas,Fazal Raziq,Nasir Ilyas,Liuxin Yang,Sharafat Ali,Amir Zada,Syedul Hasnain Bakhtiar,Yong Wang,Huahai Shen,Liang Qiao
The electrocatalytic nitrogen reduction reaction (NRR) has emerged as a promising renewable energy source and a feasible strategy as an alternative to Haber-Bosch ammonia (NH 3 ) synthesis. However, finding an efficient and cost-effective robust catalyst to activate and cleave the extremely strong triple bond in nitrogen (N 2 ) for electrocatalytic NRR is still a challenge. Herein, a FeNi@CNS nanocomposite as an efficient catalyst for N 2 fixation under ambient conditions is designed. This FeNi@CNS nanocomposite was prepared by a simple water bath process and post-calcination. The FeNi@CNS is demonstrated to be a highly efficient NRR catalyst, which exhibits better NRR performance with exceptional Faradaic efficiency of 9.83% and an NH 3 yield of 16.52 μg h −1 cm −2 in 0.1 M Na 2 SO 4 aqueous solution. Besides, high stability and reproducibility with consecutive 6 cycles for two hours are also demonstrated throughout the NRR electrocatalytic process for 12 h. Meanwhile, the FeNi@CNS catalyst encourages N 2 adsorption and activation as well as effectively suppressing competitive HER. Therefore, this earth-abundant FeNi@CNS catalyst with a subtle balance of activity and stability has excellent potential in NRR industrial applications.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
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IF 6.165
Ke Li,Hao Fang,Xiuzhi Duan,Dongshun Deng
Development of high-efficient solvents for NH 3 capture to improve the quality of atmosphere and ecological environment is a hot research topic. Deep eutectic solvents (DESs) as NH 3 absorbents can overcome some problems troubling the traditional NH 3 capture process. In this work, NH 4 SCN was paired with imidazole (Im) DESs to form low viscous DESs with dual active sites for highly efficient NH 3 absorption. The effects of absorption temperature, gas flow rate, water content, molar ratio on NH 3 absorption performance as well as physical properties of NH 4 SCN/Im DESs were systematically investigated. The results show that NH 4 SCN/Im DESs can rapidly capture NH 3 with good recycling performance, while the gas flow rate only shortens the absorption time. The NH 3 absorption capacity of NH 4 SCN/Im DESs decreased with increasing temperature and NH 4 SCN/Im molar ratio. The absorption capacity of NH 4 SCN/Im (1:2) DES reaches 9.65 mol NH 3 /kg DESs for atmospheric NH 3 . Based on 1 H NMR and IR spectroscopy analysis, the strong hydrogen bond between protic ammonium cation and NH 3 plays the major essence of efficient NH 3 capture for NH 4 SCN/Im DESs.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
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IF 7.46
Qi Hu,Zhenming Wang,Junyu Chang,Peng Wan,Jiahui Huang,Liang Feng
The accurate and rapid sensing of NH 3 at room temperature is a challenging conundrum for daily life and environment protection. In this work, we have explored an intriguing material, hollow NiO sphere composited with polyaniline (labelled as h-NiO-PANI) for NH 3 gas sensing, fabricated by growing PANI on the hollow NiO sphere derived from solvothermal synthesis and calcination. Ni-Cu glycerate is obtained via solvothermal synthesis, which is a universal way to produce uniform glycerate microspheres. During calcination, the hollow sphere is ingeniously designed by taking advantage of the outward adhesion from CuO to the inner core. Polymerization of aniline on the hollow spheres is beneficial for large specific surface area and gas adsorption. Impressively, the sensor based on h-NiO-PANI exhibits favorable response to NH 3 (ΔR/R 0 =43 % for 10 ppm, 149 s in response and 257 s in recovery), which is greatly better than the counterparts (NiO-PANI and PANI). Moreover, the sensor has also shown superb anti-interference against common volatile organic compounds (VOCs), water and humidity, along with the superior repeatability in 5 cycles and long-term stability in a week, manifesting the sensor a promising candidate in daily application. The enhanced gas sensing performance is attributed to the hollow structure and construction of p-p heterojunctions between NiO and PANI.
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CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Yiqing Zeng,Yanan Wang,Plaifa Hongmanorom,Zhigang Wang,Shule Zhang,Jiatang Chen,Qin Zhong,Sibudjing Kawi
Highly-efficient CeO 2 -TiO 2 -based catalyst is an attractive alternative to traditional V 2 O 5 -based catalysts for selective catalytic reduction of NO x by NH 3 (NH 3 -SCR). Herein, we construct an efficient and stable P-doped CeO 2 /TiO 2 ( y CeTi-P x ) catalyst by dispersing CeO 2 on strongly acidic and highly stable mesoporous P-doped TiO 2 (Ti-P x ). The characteristic structure of Ti-P x causes highly dispersed CeO 2 , strong active component-support interaction, and abundant surface active oxygen and acid sites on CeTi-P catalyst. Therefore, y CeTi-P x catalyst exhibits much higher catalytic activity than y CeTi catalyst at temperature of 200–450 °C. The y CeTi-P x catalysts show high activity in the presence of H 2 O and strong resistance to H 2 O + SO 2 at medium-high temperature, implying that they have great industrial application prospects. Different P/Ti ratio and CeO 2 loading content were investigated. Excessive P doping can block the Ce 4+ /Ce 3+ redox couple, and suppress redox sites on y CeTi-P x catalyst. Additionally, increasing CeO 2 content can reduce the NH 3 capacity of y CeTi-P x catalyst. By controlling the P/Ti ratio and CeO 2 loading content, surface acid sites and redox sites on y CeTi-P x catalyst can be balanced to obtain the best catalytic activity. This work demonstrates a feasible method in adjusting acid sites and redox sites on CeTi catalyst, which ultimately contributes to the new design of CeO 2 -TiO 2 -based catalyst.
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RSC Advances
·
2022
·Vol. 12
·期 51
·33056-33063
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IF 4.036
Bo Huang,Zhihua Zhao,Pu Chen,Baocang Zhou,Zhuo Chen,Yu Fu,Hongyu Zhu,Chen Chen,Shuaiwen Zhang,Anbiao Wang,Pu Shi,Xiaoqing Shen
Ammonia (NH3) is a common air pollutant and is a biomarker for kidney disease. Therefore, the preparation of ammonia gas sensors with high sensitivity, good selectivity and low operating temperature is of great importance for health protection. Using the in situ electrostatic self-assembly approach, a chemoresistive gas sensor based on Co(OH)2/Ti3C2Tx hybrid material was created in this study. The prepared samples were characterized by XRD, XPS, TEM, BET and other testing methods for structure, surface topography and elements. These samples were fabricated into sensors, and the gas sensing properties of the materials were investigated under different test conditions. The results show that the gas response value of the C/M-2 sensor is up to about 14.7%/100 ppm, which is three times the response value of the sensor made of pure MXene to NH3. In addition, the Co(OH)2/Ti3C2Tx hybrid sensors exhibit excellent repeatability, high sensitivity under low concentration (less than 5 ppm), fast response/recovery time (29 s/49 s) and long-time stability, which indicates their promising utility in the IoT field.
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Small
·
2023
·
IF 13.3
Heng Guo,Peng Yang,Yuantao Yang,Haoran Wu,Fengying Zhang,Zhen-Feng Huang,Guidong Yang,Ying Zhou
Ambient electrocatalytic nitrogen (N 2 ) reduction has gained significant recognition as a potential substitute for producing ammonia (NH 3 ). However, N 2 adsorption and *NN protonation for N 2 activation reaction with the competing hydrogen evolution reaction remain a daunting challenge. Herein, a defect-rich TiO 2 nanosheet electrocatalyst with PdCu alloy nanoparticles (PdCu/TiO 2−x ) is designed to elucidate the reactivity and selectivity trends of N 2 cleavage path for N 2 -to-NH 3 catalytic conversion. The introduction of oxygen vacancy (OV) not only acts as active sites but also effectively promotes the electron transfer from Pd-Cu sites to high-concentration Ti 3+ sites, and thus lends to the N 2 activation via electron donation of PdCu. OVs-mediated control effectively lowers the reaction barrier of *N 2 H and *H adsorption and facilitates the first hydrogenation process of N 2 activation. Consequently, PdCu/TiO 2−x catalyst attains a high rate of NH 3 evolution, reaching 5.0 mmol g cat. −1 h −1 . This work paves a pathway of defect-engineering metal-supported electrocatalysts for high-efficient ammonia electrosynthesis.
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JOURNAL OF THE ENERGY INSTITUTE
·
2023
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IF 5.7
Yun Shi,Tingman Zhao,Jiada Du,Bo Feng,Qiuqi Tang,Shengdao Shan,Min Zhang,Qun Wang,Jingkai Zhao
A highly efficient CeO x -BC 0.6 (BC: biochar. 0.6: mass ratio of Ce/(BC + Ce)) catalyst was prepared by air oxidation for low temperature NH 3 selective catalytic reduction of NO x . The catalytic performance, characterization and reaction mechanism of the CeO x -BC 0.6 were investigated. The results showed that NO x conversion and N 2 selectivity of CeO x -BC 0.6 catalyst obtained by calcining in air were above 90 % at 150–300 °C and 100,000 h −1 . The surface oxygen groups, acid sites and oxygen vacancies were generated by air oxidation treatment, which promoted the adsorption and activation of reactants. NH 3 and NO x were adsorbed on the catalyst surface in the form of NH 4 + , NH 3 + , nitrite and nitrate adspecies. The redox cycles of ketonic carbonyl/phenol (C O/C–OH) pairs and Ce 4+ /Ce 3+ pairs were responsible for the activation of NH 3 and NO x . NH 2 NO and NH 4 NO 2 were the main active intermediates. The reaction of NH 3 selective catalytic reduction of NO x over CeO x -BC 0.6 mainly followed Eley-Rideal mechanism. These results will promote the understanding of mechanism of NH 3 selective catalytic reduction of NO x for biochar-based catalyst prepared by air oxidation.
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JOURNAL OF SOLID STATE CHEMISTRY
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2023
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IF 3.3
Yuting Hu,Ting Cheng,Zhaozhong Jiang,Kai Qin,Han He,Chengzhu Zhu
Fe-MIL-101-NH 2 was prepared by solvothermal method with ferric nitrate and 2-Aminoterephthalic Acid (DBC-NH 2 ), and Fe-MIL-101-NH 2 as precursor was calcined to prepare α-Fe 2 O 3 catalyst. The optimum synthesis condition and the NO conversion efficiency of α-Fe 2 O 3 were systematically investigated, and its crystallinity, micro-morphology and surface acidity were characterized. The results showed that α-Fe 2 O 3 over calcination at 400 °C for 1 h had excellent catalytic activity, SO 2 tolerance, water resistance, and stability. When an initial NO concentration of 500 ppm, the gas hourly space velocity (GHSV) of 35000 h −1 , and a reaction temperature of 350 °C, the NO conversion efficiency of α-Fe 2 O 3 remained above 90 %. The crystal structure of the catalyst was α-Fe 2 O 3 which retained the original octahedral morphology of Fe-MIL-101-NH 2 and increased a lot of new pores, leading to more abundant Lewis acid sites for promoting NO conversion efficiency.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Min Zheng,Zhihao Yan,Xingbang Hu,Zhuoheng Tu,Youting Wu
It has been of long concern that the separation and recovery of NH3 from industrial processes, in addition to attracting huge economic interest, also reduce environmental pollution. So, it is very urgent to develop novel absorbents for highly efficient capture of NH3. In this study, several novel tetrazole (TetrZ)-based binary deep eutectic solvents (DESs) were formed by mixing TetrZ with 1,2,3-triazole (1,2,3-Tri), ethylene glycol (EG), 2-morpholinoethanol (2-Mor), or N-methyldiethanolemine (MDEA) to absorb NH3. TetrZ + 1,2,3-Tri (1:4, mole ratio) not only exhibits higher NH3 absorption ability of 0.239 gNH3·gDES–1 than that of most absorbents reported to date at 313.15 K and 101.3 kPa, but also shows elevated selectivities of 592.7 for NH3/CO2, 654.5 for NH3/N2, and 1033.7 for NH3/O2. Meanwhile, TetrZ + 1,2,3-Tri (1:4) can be reused 10 times with good absorption capacity retained. Additionally, the solubility data of NH3 were correlated by the reaction equilibrium thermodynamic model. The NMR and FTIR spectroscopic characterizations were also used to study the absorption mechanism, and quantum chemistry calculation was utilized to further investigate the interactions between NH3 and DESs from an atomic level perspective. The DESs developed in the present work have the potential to capture NH3 sustainably, owing to their high solubility, superior selectivity, and desirable reversibility.
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JOURNAL OF PHYSICS D-APPLIED PHYSICS
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2023
·Vol. 56
·期 49
·495103
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IF 3.4
Yujiao Ma,Yuzhou Sun,Zihan Zhang,Haokai Zhao,Haifeng Gao,Qing Zhou,Wenbo Li,Xiaoyun Teng,Chao Gao,Wei Yu
In this paper, the open-circuit voltages (VOC) of Cu2ZnSn(S,Se)4 (CZTSSe) solar cells were improved by soaking the CZTSSe films in Cd/NH3 solutions before the deposition of buffer layers. The effects of Cd/NH3 soaking on the properties of CZTSSe films and solar cells were investigated in depth. We found Cd/NH3 soaking can promote downward band bending of the CZTSSe layer at the surface region. In addition, the Cd/NH3 soaking can eliminate the deep level acceptor in CZTSSe and decrease the density of the defects at the absorber/buffer interface. These effects can significantly reduce the carrier recombination in the depletion region of CZTSSe solar cells. As a result, the VOC of CZTSSe solar cells were increased from ∼460 mV to ∼480 mV, the efficiency of the best CZTSSe solar cell was increased from 10.2% to 11.6% by the Cd/NH3 soaking process.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Ruyi Yang,Jinniu Zhang,Jia Liu,Gang Li,Yu Qiao,Xinyi Zhang,Jianzhi Gao,Hongbing Lu
The rational design of sensing materials with distinct morphologies and compositions is important to construct outstanding flexible gas sensors. Herein, a mesh polyaniline (PANI)/Ti 3 C 2 T x composite nanofiber-based flexible sensor was constructed by electrospinning of PANI and few-layer Ti 3 C 2 T x nanosheets . Sensing results indicated that this novel PANI/Ti 3 C 2 T x flexible sensor demonstrated much higher NH 3 sensing response (2.3-fold improvement @ 20 ppm) in comparison with the sensor based on pure PANI nanofibers at 25 °C. Under different bending angles (maximum compression of 150°) and different bending times (maximum bending of 3200 times), the PANI/Ti 3 C 2 T x flexible sensor maintained steady sensing behavior towards 20 ppm NH 3 , which reflected its good flexible bending stability. The PANI/Ti 3 C 2 T x flexible sensor also exhibited good selectivity, repeatability, as well as good long-term stability. The improvement of NH 3 sensing properties can be ascribed to the formation of Schottky junctions between PANI and Ti 3 C 2 T x nanosheets, improved protonation degree of PANI, and the special three-dimensional mesh fiber structure. Our work revealed that the PANI/Ti 3 C 2 T x composite nanofibers with interconnected mesh fiber structure have great potential to construct flexible NH 3 sensors.
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JOURNAL OF THE SCIENCE OF FOOD AND AGRICULTURE
·
2023
·
IF 4.1
Yingnan Liu,Fei Tong,Yingran Xu,Yunyun Hu,Wenya Liu,Zan Yang,Zhenyu Yu,Guoyuan Xiong,Yibin Zhou,Yaqing Xiao
BACKGROUND Active and smart food packaging based on natural polymers and pH-sensitive dyes as indicators has attracted widespread attention. In the present study, an antioxidant and amine-response color indicator film was developed by incorporating bilirubin (BIL) into the κ-carrageenan (Carr) matrix. RESULTS It was found that the introduction of BIL had no effect on the crystal/chemical structure, water sensitivity and mechanical performance of the Carr-based films. However, the barrier properties to light and the thermal stability were significantly improved after the addition BIL. The Carr/BIL composite films exhibited excellent 1,1-diphenyl-2-picryl-hydrazyl (i.e. DPPH)/2,2′-azino-bis-(3-ethylbenzothiazoline-6-sulfonic acid) (i.e. ABTS) free radical scavenging abilities and color responsiveness to different concentrations of ammonia. The application assay reflected that the Carr/BIL 0.0075 film was effective in delaying the oxidative deterioration of shrimp during storage and realizing the color response of its freshness through the change of b * value. CONCLUSION Active and smart packaging films were successfully prepared by incorporating different contents of BIL into the Carr matrix. The present study helps to further encourage the design and development of a multi-functional packaging material. © 2023 Society of Chemical Industry.
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