ELECTROCHIMICA ACTA
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2024
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IF 5.5
Daming Feng,Lixue Zhou,Chang Liu,Hui Li,Yusheng Zhang,Yali Yao,Tianyi Ma
Electrocatalytic nitrogen reduction reaction (NRR) for the synthesis of ammonia (NH 3 ) is one of the green and mild methods of artificial nitrogen fixation, promising as an alternative to replace the existing industrial process. Under the requirements of green chemistry and sustainable development, the design and development of highly active and stable electrocatalysts is very important for improved synthesis performance. Mimicking from the natural nitrogenase, Fe and Mo based catalysts have attracted much attention due to their superior catalytic performance for N 2 adsorption and activation. In this work, an interfacial engineering strategy has been used to prepare a Fe, Mo-bimetallic electrocatalyst for the electrosynthesis of NH 3 . In detail, the pre-pyrolyzed biochar-based Fe 2 O 3 composites were decorated with nano-flowered MoS 2 /MoO 2 hybrids by a solvothermal process (MoS 2 /MoO 2 @Fe 2 O 3 /BC). As confirmed by the extensive characterization, the further modification not only introduced functional counterparts into the electrocatalysts but also regulated the morphology of the nanostructure. The electrochemical tests showed that the highest NH 3 yield rate of MoS 2 /MoO 2 @Fe 2 O 3 /BC was 4.87 μg h − 1 cm −2 and highest FE was 16.5% in 0.1 M Na 2 SO 4 . The catalytic stability and durability were also presented in the longtime electrolysis and cycling experiments. The improved catalytic performance of decorated catalyst, as evidenced by the comparison with Fe 2 O 3 /BC, is attributed to the increased electrocatalytic active area, the moderated hydrophilicity, and the synergistic effect of Fe, Mo-bimetallic active sites. This study provides a new perspective for the design and development of low-cost transition metal complexes as electrocatalysts for nitrogen reduction reactions.
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RSC Advances
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2024
·Vol. 14
·期 17
·12225-12234
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IF 3.9
Zhixuan Wu,Zhengai Chen,Zhixiang Deng,Ning Dai,Yan Sun,Meiying Ge
In this work, a high-performance room-temperature ammonia (NH3) gas sensor based on Pt-modified WO3–TiO2 nanocrystals was synthesized via a two-step hydrothermal method. The structural properties were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The 10 at% Pt@WO3–TiO2 nanocrystals present the highest NH3 sensing performance at room temperature. Compared with the nanocrystals without Pt modification, the sensitivity of the Pt@WO3–TiO2 sensor is tenfold higher, with the lowest concentration threshold reaching the 75 ppb level. The response is approximately 92.28 to 50 ppm, and response and recovery times are 23 s and 8 s, respectively. The improved sensing was attributed to a synergetic mechanism involving the space charge layer effect and Pt metal sensitization, enhancing the electron transfer efficiency, oxygen vacancy and specific surface area. This study is expected to guide the development of high-performance room-temperature ammonia sensors for clinical breath testing.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Xinyu Han,Kaijie Liu,Mengyao Bian,Zhaoxu Yuan,Yannan Li,Yunlong Zhang,Xiangguang Yang,Yibo Zhang
Despite SO 2 being recognized as a catalyst poisoning substance, a trace amount can enhance the acidity of the NH 3 -SCR (selective catalytic reduction) catalyst, which facilitates NH 3 adsorption and accelerates the reaction rate according to the Eley-Rideal mechanism. In this study, monoatomically dispersed Ce atoms were doped into the MoTiO x lattice to regulate the quantity and distribution of sulfate. This regulation was achieved by leveraging the stronger affinity of SO 2 to Ce, thus maximizing the acidifying effect of SO 2 to boost the NH 3 -SCR performance of the catalyst. The catalyst demonstrated the ability to maintain over 80 % NO x conversion for at least 144 hours in the presence of high concentration SO 2 (250 ppm). A detailed examination of the surface dynamics after SO 2 introduction revealed that NH 4 (SO 4 ) 2 , formed on the surface, converted to NH 4 HSO 4 . The decomposition of NH 4 HSO 4 extracted lattice oxygen from the catalyst, leading to an increase in oxygen vacancies on the catalyst surface as the duration of SO 2 exposure increased. The surface-adsorbed oxygen, brought about by these oxygen vacancies, was readily activated, which promoted the dehydrogenation process of NH 3 and the progression of NH 3 -SCR. Further, based on the discovery of the unique phenomenon and mechanism of NH 4 HSO 4 decomposition that generates oxygen vacancies, gases containing poisonous SO 2 were utilized for the pretreatment of the catalyst to optimize its surface and enhance its sulfur resistance (fighting poison with poison). The results demonstrated that the pretreated catalyst rapidly achieved optimal NO x conversion and maintained catalytic stability for over 240 h even in the presence of 250 ppm SO 2 without any decrease in activity. This research innovatively leveraged the poisonous SO 2 to optimize the catalyst's surface, thereby achieving higher catalytic performance and sulfur resistance, which offers valuable insights into the design of novel sulfur-resistant catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Shuyi He,Zheguan Lin,Jie Shi,Linyu Zhou,Qingyan Cui,Tiesen Li,Jiangyong Liu,Yuanyuan Yue
For traditional strategies to construct SO 2 and H 2 O co-resistant systems in low-temperature NH 3 selective catalytic reduction (NH 3 -SCR) catalysts, the primary challenge lies in mitigating the partial loss of redox activity at active sites. Herein, we present an approach to construct a protective system based on interface engineering principles, effectively safeguarding Cu active sites in ZnO/FeCu-SSZ-13 under SO 2 and H 2 O exposure. The core innovation stems from the creation of a strong interface effect originated from Zn-O-Al bonds formed between ZnO and the framework Al on the FeCu-SSZ-13 surface. This interface effect can regulate the electronic structure of Zn O bonds on ZnO component, producing abundant basic sites around the Cu active sites, enabling the preferential adsorption of SO 2 and its oxidation into ZnSO 4 , thereby virtually eliminating the redox ability loss of Cu active sites. As a result, ZnO/FeCu-SSZ-13 achieves exceptional low-temperature NH 3 -SCR performance, maintaining over 90 % NO x conversion even in the presence of SO 2 and H 2 O. Our work opens a new avenue for developing low-temperature NH 3 -SCR catalysts with desired SO 2 and H 2 O resistance, offering valuable insights for advancing catalytic performance in challenging reaction conditions.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 11
·1-13
·
IF 5.3
Zhao Zhihua,Su Zijie,Lv Zhenli,Shi Pu,Jin Guixin,Wu Lan
Bi 2 S 3 /Ti 3 C 2 T x nanomaterials were successfully prepared through a simple hydrothermal method. Various methods were used for their characterization, including XRD, XPS, SEM, EDS, and BET, along with testing their gas-sensing properties. The results showed that the response value to 100 ppm ammonia at room temperature reached 107%, which was 14.1 times higher than that of pure few-layer MXene. After undergoing anti-humidity interference testing, we observed that Bi 2 S 3 /Ti 3 C 2 T x exhibited a higher response value in real-time monitoring of ammonia as humidity increased. Specifically, under 90% humidity conditions, its response value reached 1.32 times that of normal humidity conditions. This exceptional moisture resistance ensures that the sensor can maintain stability, and even exhibit superior performance, in harsh environments. Therefore, it possesses excellent selectivity, high-moisture-resistance, and long-term stability, making it significant in the field of medical and health monitoring. Graphical abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Qinyu Zhou,Chong Tan,Tianfa Tang,Yu Wang,Siyuan Li,Meilin Tao,Hongliang Zhang,Liu Yang,Changjin Tang
The occurrence of NH 3 over-oxidation represents one intractable challenge for the effective application of NH 3 -SCR technology. Herein, a rational NO x activation strategy was innovatively proposed to counteract NH 3 over-oxidation during high temperature NH 3 -SCR. As a proof of concept, the hybrid catalyst of CeO 2 -ZSM-5 was explored. It was shown that the activity of CeO 2 in NH 3 -SCR was profoundly improved via physically mixing with ZSM-5, achieving more than 85 % NO at 500 °C, in sharp contrast to the negative NO conversion present for pristine CeO 2 . Comprehensive characterizations from NH 3 -TPD, NO-TPD and in situ DRIFTS verified the negligible modification of NH 3 oxidation but significant alteration of surface NO x . Due to the facile NO x activation, the reaction of NH 3 + NO x overwhelms that of NH 3 + O 2 , leading to the obtainment of excellent high temperature NH 3 -SCR performance. The novel strategy reported here is expected to provide valuable guidance for designing NH 3 -SCR catalysts with superior high temperature performance.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Weili Ye,Jin Li
Ammonia (NH 3 ) is a common but potentially hazardous gas that may cause inflammation of the lungs or other respiratory illnesses when exposed to high levels of NH 3 for extended periods. Therefore, preparing a gas sensor for real-time monitoring of NH 3 gas at room temperature is of great practical significance. In this paper, a Zn 2 SnO 4 /ZnO (ZZ) metal-oxide-semiconductor gas sensor with high response to NH 3 gas, low cost, easy fabrication, and high selectivity was successfully prepared by using a one-pot hydrothermal method. It was discovered that the content of the mineralizer NaOH serves to regulate the morphology of the samples. The results indicated that this method facilitated a more favorable formation of the n-n type heterojunction between Zn 2 SnO 4 and ZnO, leading to a substantial improvement in the sensor's sensitivity to NH 3 gas. Upon the addition of 3.75 mol/L NaOH, the Zn 2 SnO 4 and ZnO contents in the Zn 2 SnO 4 /ZnO (ZZ-3) samples were approximately equivalent. As a result, under the n-n heterojunction and synergistic interaction, the sensor demonstrated a significantly higher response (1756.1) to 500 ppm of NH 3 at RT, compared to the response values of the pure Zn 2 SnO 4 sample (24.3) and pure ZnO (23.6). Moreover, compared with the response values to other common harmful gases (500 ppm) in daily life, the response to NH 3 was approximately 10.7–1393.7 times higher. Meanwhile, the ZZ-3 samples also exhibit excellent long-term stability. This work provides an idea of using NaOH to modulate the material morphology for the preparation of gas-sensitive sensors.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Kaidi Wu,Hongfeng Chai,Kaichun Xu,Marc Debliquy,Chao Zhang
High working temperature and the insufficient limits of detection limit the broad applications of semiconductor chemiresistive gas sensors. Herein, pure Bi 2 MoO 6 nanosheets and a series of one-dimensional/two-dimensional (1D/2D) multi-walled CNTs/Bi 2 MoO 6 nanocomposites were developed via a facile hydrothermal route for room-temperature ammonia monitoring. The as-synthesized samples were characterized by various analytical techniques. 0.5 wt% MWCNTs/Bi 2 MoO 6 nanocomposites showed the best sensing properties to 10–50 ppm NH 3 , including low limit of detection (157 ppb), high response (R a /R g = 44.2 @ 50 ppm), good selectivity, reproductivity, and anti-humidity sensing ability. The enhanced gas sensing mechanism was proposed based on the synergetic effect of high-energy crystal facets, modified surface characteristics and p-n heterojunction . Density functional theory (DFT) studies were also carried out to further clarify the gas sensing mechanisms. This work provides a practical approach to design and fabricate high-precision gas sensors working at room temperature .
研究领域:
材料科学
·
传感器技术
·
化学工程
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ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Jiali Liu,Xianbiao Wang,Yangyang Zhao,Yongfei Xu,Yang Pan,Shaojie Feng,Jin Liu,Xianhuai Huang,Huanting Wang
Radioactive U(VI) in nuclear wastewater is a global environmental pollutant that poses a great threat to human health. Therefore, it is of great significance to develop a U(VI) sensor with desirable sensitivity and selectivity. Inspired by electron-donating group modification for enhancement of binding affinity toward U(VI), we report an amine group functionalization of UiO-66-NH2, using a low-cost, environmentally friendly, and low-temperature NH3 plasma technique as a fluorescence switching nanoprobe for highly sensitive and selective detection of U(VI). The resulting amine-functionalized UiO-66-NH2 (LTP@UiO-66-NH2) shows dramatically enhanced fluorescence emission and selective sensitivity for U(VI) on the basis of the quenching effect. The quenching efficiency increases from 58 to 80% with the same U(VI) concentration (17.63 μM) after NH3 plasma functionalization. As a result, the LTP@UiO-66-NH2 has the best Ksv (1.81 × 105 M–1, 298 K) and among the lowest LODs (0.08 μM, 19.04 ppb) compared with those reported in the literature. Intraday and interday precision and application in real environment experiments indicate stable and accurate U(VI) detection performance. Fluorescence lifetime and temperature-dependent detection experiments reveal that the quenching mechanism belongs to the static quenching interaction. The highly selective fluorescence detection is attributed to the selective binding of U(VI) by the rich functionalized amine groups of LTP@UiO-66-NH2. This work provides an efficient fluorescence probe for highly sensitive U(VI) detection in water, and a new strategy of tailored plasma functionalization for developing a practical MOF sensor platform for enhanced fluorescence emission, sensitivity, and selectivity for detecting trace amounts of radioactive species in the environment.
研究领域:
环境科学
·
材料科学
·
放射化学
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Nature Communications
·
2026
·
IF 18.1
Guo Xuewen,Hu Yongji,Wu Xiaoyi,Shen Yuesong
H 2 O and SO 2 poisoning of cerium-manganese oxide catalysts remains a critical challenge for low-temperature selective catalytic reduction of nitrogen oxides by NH 3 . Here we show that Ti doping of CeO 2 induces lattice contraction and structural distortion, promoting the generation of oxygen vacancies, active oxygen species, and stable Ce-O-Ti interfaces. These strain-engineered structural modifications enhances surface Lewis acidity and triggers a downshift of the d-band center, collectively improving low-temperature catalytic activity and resistance to H 2 O/SO 2 poisoning. The optimized Ce 8 MnTi 2.5 O x catalyst achieves over 90% nitrogen oxides removal across a 150–335 °C temperature range. Under 5 vol.% water and 100 ppm SO 2 , it maintains over 98% efficiency for 12 h at 210 °C. Furthermore, during stepwise heating from 150 °C to 240 °C with 5 vol.% H 2 O and 200 ppm SO 2 , initial activity suppression below 180 °C is fully reversed at or above 210 °C, demonstrating temperature-driven regeneration. This study introduces a strain-engineering strategy for designing robust catalysts for low-temperature nitrogen oxides removal.
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JOURNAL OF ELECTRONIC MATERIALS
·
2026
·
IF 2.8
Zhang Fan,Zhang Jinshun,Li Xu,Wang Qingji
Polyaniline (PANI) is regarded as a prospective sensing material for room-temperature NH 3 detection owing to its high sensitivity and selectivity. In this study, WO 3 nanoflowers were prepared via a simple chemical bath deposition method, and PANI/WO 3 heterojunctions were subsequently fabricated through an in situ polymerization process. To evaluate the contribution of the heterojunction to gas-sensing performance, four sensors with different composite ratios were constructed. Among them, the optimized PW1-2 sensor exhibits a response of 3.8–100 ppm NH 3 at room temperature, which is 1.6 times higher than that of pure PANI. Notably, it achieves an ultrafast response time of only 26 s, representing an 8.8-fold improvement over pure PANI (230 s), along with near-complete desorption capability. Furthermore, PW1-2 demonstrates excellent humidity resistance, with stable responses ranging from 3.7 to 3.97 under 40–80% relative humidity. Comprehensive characterization by x-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy TEM, x-ray photoelectron spectroscopy (XPS), Raman spectroscopy, thermogravimetric analysis (TGA), and Brunauer–Emmett–Teller (BET) analysis reveals that PANI nanofibers uniformly wrap around WO 3 nanoflowers, forming p–n heterojunctions at the interface. XPS analysis shows that PW1-2 possesses the highest protonation degree (51.88%), which correlates with its superior sensing performance. Unlike conventional PANI/WO 3 composites, the enhanced performance is not primarily attributed to specific surface area or porosity but rather to the synergistic effect of morphological characteristics and heterojunction formation. Compared with previously reported PANI/WO 3 sensors, our PW1-2 sensor offers significantly faster response, better humidity tolerance, and complete desorption. This work provides a promising strategy for designing high-performance, humidity-resistant room-temperature NH 3 sensors. Graphical
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SENSORS AND ACTUATORS B-CHEMICAL
·
2026
·
IF 8.3
Zheng Wang,Weiwei Meng,Ling Wang,Yuehua Li,Xu Li,Lei Dai
Cu-doped Bi 4 V 2 O 11 enabled medium-temperature mixed-potential NH 3 sensing. • Measurable NH 3 response appeared at 200°C, with optimum performance at 400°C. • Sensitivity increased with the conductivity of the solid electrolyte. The development of reduced operating temperature mixed-potential NH 3 sensors is hindered by insufficient ionic conductivity of conventional solid electrolytes at moderate temperatures. Here, a series of Cu-doped Bi 4 V 2-x Cu x O 11-δ (x = 0, 0.1, 0.2, 0.3) solid electrolytes were synthesized via a solid-state method to enhance oxygen ion transport. A mixed-potential NH 3 sensor was fabricated utilizing InVO 4 as the sensing electrode. Among the compositions, Bi 4 V 1.8 Cu 0.2 O 11-δ exhibited the highest conductivity, showing an over one order of magnitude increase at 400℃ compared with the undoped electrolyte. The resulting sensor showed a response to 10~300 ppm NH 3 over 200~550℃ and achieved a maximum sensitivity of −97.9 mV/decade at 400℃. Impedance/polarization analysis indicated that the sensing enhancement tracked the improved ionic transport of the Cu-doped electrolyte and followed the mixed-potential mechanism. This study highlights Bi 4 V 2-x Cu x O 11-δ -type electrolytes as promising electrolytes for moderate-temperature solid-electrolyte NH 3 sensing. Download: Download high-res image (148KB) Download: Download full-size image
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