SENSORS AND ACTUATORS B-CHEMICAL
·
2026
·
IF 8.3
Xiaoqing Jiang,Feng Qiu,Jie Wang,Chu Cheng,Panhui Yang,Tao Yuan,Jiawen Jian,Xianwang Ye,Jie Zou
Yttria-stabilized zirconia (YSZ)-based ammonia (NH 3 ) sensors offer high-temperature stability and real-time monitoring capabilities for environmental protection. However, these promising sensors suffer from low sensitivity governed by the sensing electrode (SE), where surface Lewis acidity and microstructural properties regulate the selective adsorption and activation of NH 3 . In this work, TiNb 2 O 7 with exposed Ti 4 + /Nb 5+ Lewis-acidic sites was first employed as the SE for a YSZ-based mixed-potential NH 3 sensor, with its microstructure optimized to enhance sensing performance. The sensor exhibited a superior response of −202.41 mV to 200 ppm NH 3 with a sensitivity of −119.27 mV/decade at 600℃, attributed to the synergy between exposed Ti 4+ /Nb 5+ Lewis-acidic sites and optimized triple-phase boundaries accessibility. Furthermore, the sensor demonstrated high selectivity against common interfering gases (NO, NO 2 , C 3 H 6 , and CH 4 ) and robust stability over 30 days.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2026
·
IF 8.3
Hao Wu,Xieraili Maimaitiyiming
Ammonia (NH 3 ) and carbon monoxide (CO) are typical toxic gases found in industrial emissions and indoor environments, posing serious threats to human health and ecological stability. Consequently, developing sensitive, highly selective, and multifunctional gas sensors holds significant practical importance. This study constructed sensors based on semiconducting single-walled carbon nanotubes (sc-SWCNTs) through non-covalent coating with azo polymers, focusing on investigating the impact of azo compound cis-trans isomerization on carbon nanotube separation efficiency and gas sensing performance. Results indicate that both isomers exhibit excellent sc-SWCNT separation capability, yielding sc-SWCNTs with purity exceeding 99.9%; sensors fabricated from the two composite materials exhibit significant differences in transient response performance under 35 s exposure conditions. At a 1 ppm NH 3 concentration in air, the trans-PFAAB/sc-SWCNTs and cis-PFAAB/sc-SWCNTs sensors exhibited response values of 12.1% and 3.8%, respectively. When exposed to 1 ppm CO in air, their response values were 6.8% and 4.7%, respectively. This study demonstrates that the trans configuration of azo groups confers greater application advantages in azo polymer/sc-SWCNTs composite sensors, offering novel insights for developing high-performance polymer/semiconducting single-walled carbon nanotube composite sensors.
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ACS Catalysis
·
2025
·
IF 13.1
Yanfei Liu,Zhang Liu,Yi Yu,Chun Du,Jie Xu,YaoHui Dun,Chengxiong Wang,Yunkun Zhao,Aimin Zhang,Fudong Liu,Wei Li,Rong Chen,Bin Shan
Isolated atom catalysts face challenges in structure-sensitive reactions due to their oxidic electronic states and the lack of ensemble sites. A strategy employing the coupling between the coordination environment and adsorbate species is developed to overcome these limitations by constructing PtCu heteroatom ensembles, which unleashes the latent power of isolated Pt atoms for NH3–SCO reactions. Through the integrated exploration of theoretical calculations and experimental studies, we elucidate the pivotal role of structural sensitivity and isolated Pt coordination environments in shaping the electronic structure of Pt and its interaction with adsorbates. Our work reveals the Cu–Pt1–Cu atomic site as a breakthrough configuration, displaying unprecedented catalytic activity and selectivity in NH3–SCO reactions, far surpassing traditional Pt-based catalysts. Remarkably, the dispersed Cu–Pt1–Cu heteroatom ensemble achieves a turnover frequency of 0.29 s–1 at 150 °C, being the highest among Pt-based catalysts, and outperforming representative Pt1 SACs by an impressive 6 orders of magnitude, while its N2 selectivity remains above 89.7%. This heightened performance is attributed to its distinctive electronic properties, characterized by free-atom-like metallic Pt electronic orbitals embedded within a bulk like Pt1–Cun ensemble structure.
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Catalysts
·
2026
·Vol. 16
·期 1
·
IF 4
Xin Liu,Jinshan Zhang,Tao Sun,Hisahiro Einaga,Hajime Hojo,Pengwei Huo
A series of novel Ce-modified MnCoAl layered double oxides (Ce/MCA LDOs) were prepared using solvothermal and impregnation methods for NH3-SCR denitration. Various characterizations, such as X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and H2temperature-programmed reduction (H2-TPR) were used to investigate their structural properties and the mechanism of ammonia selective catalytic reduction (NH3-SCR). The incorporation of Ce was found to effectively integrate into the LDO framework and enhance the catalytic activity over a wide temperature window. Moreover, the thermal stability and resistance of H2O and SO2were evaluated. In situ DRIFTS studies revealed that the reaction follows both the “Langmuir–Hinshelwood” (L–H) and “Eley–Rideal” (E–R) mechanisms. This work provides systematic insights into the design of LDO-based catalysts, demonstrating their potential for practical application in denitration.
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Journal of Central South University
·
2026
·Vol. 32
·期 11
·4248-4259
·
IF 4.4
Wang Jia-yi,Liu Xin-li,Wu Zhuang-zhi,Wang De-zhi
Eco-friendly electrocatalytic nitrogen reduction reaction (NRR) is aimed to replace the traditional polluting industrial process, but NRR needs electrocatalysts with high selectivity and activity to boost desired NH 3 yield rate and Faradic efficiency (FE). In this work, high-entropy sulfides (HES) (FeCoNiMoM)S x (M=Cr, Cu, Mn) were synthesized via a two-step solvothermal method. The optimized composition for HES is (FeCoNiMoCr)S x , with promising NRR performance that NH 3 yield rate reached 47.97 µg/(h·mg cat ) at −0.7 V vs RHE and FE was 26.1% at −0.4 V vs RHE. Comprehensive characterization and electrochemical testing were performed to investigate the effects of the metal component on NRR performance. It reveals that (FeCoNiMoCr)S x shows more intense charge transport, more electrocatalytic active sites, higher selectivity, etc, resulting from the electron transport and element synergy of HES. Also, it is proved to have targeted NRR selectivity and limiting competitive hydrogen evolution reaction. The results offer promising guidance for further improving the NRR electrocatalysts based on transition elements.
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Applied Sciences-Basel
·
2018
·Vol. 8
·期 12
·
IF 1.689
Xinbo Zhu,Yaolin Wang,Yu Huang,Yuxiang Cai
In this work, a series of Ce-W-Ti catalysts were synthesized using a solution combustion method for the selective catalytic reduction (SCR) of NO with NH3at low temperatures. The reaction performance of NH3-SCR of NO was significantly improved over the Ce-W-Ti catalysts compared to Ce0.4Ti and W0.4Ti catalysts, while Ce0.2W0.2Ti showed the best activity among all the samples. The Ce0.2W0.2Ti catalyst exhibited over 90% removal of NO and 100% N2selectivity in the temperature range of 250–400 °C at a gas hourly space velocity (GHSV) of 120,000 mL·g−1·h−1. The Ce-W-Ti catalysts were characterized using N2adsorption-desorption, X-ray diffraction, X-ray photoelectron spectrometry and temperature programmed desorption of NH3to establish the structure-activity relationships of the Ce-W-Ti catalysts. The excellent catalytic performance of the Ce0.2W0.2Ti catalyst could be associated with the larger specific surface area, highly dispersed Ce and W species, increased amount of surface adsorbed oxygen (Oads) and enhanced total acidity on the catalyst surfaces.
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CATALYSIS LETTERS
·
2024
·Vol. 154
·期 8
·4378-4388
·
IF 2.3
Zheng Jiahao,Zhang Shule,Zeng Yiqing,Li Mengyu,Li Xiang,Zhong Qin
Simultaneous desulfurization and denitration by using activated coke is one of the most competitive technologies for cleaning low-temperature steel flue gases. The key to denitration performance relies on the regulation of active groups on the catalyst. In this work, the carboxyl and lactone groups with (NH 4 ) 2 S 2 O 8 oxidation and thermal treatment were found to mainly determined the catalytic activity. The results showed that (NH 4 ) 2 S 2 O 8 -treated AC catalyst improved denitration activity at low temperatures, which was attributed to the increase in oxygen-containing groups of the AC, the thermal treatment enhanced the low-temperature activity while reduced the performance in (210–240 ℃). According to the characterization results and conformational relationship analysis, we revealed that the adsorption and activation of NH 3 mainly depended on carboxyl groups during the middle-temperature range (210–240 ℃) NH 3 –SCR. Based on the advantage of middle-temperature denitration activity of modified activated coke, the carboxyl groups on activated coke were the most important active sites for the NH 3 –SCR reaction. Moreover, lactone groups, improved the denitration performance via promoting NO oxidation at low-temperatures range (120–150 ℃). However, the presence of only lactone groups in the 210–240 ℃ is not beneficial for the further promotion for denitration activity. This work initially reveals the decisive role of carboxyl and lactones groups of activated coke for the low-temperature NH 3 -SCR reaction, and guides the industrial arrangement of oxidation-modified AC as denitration catalyst. Graphical
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CATALYSIS TODAY
·
2020
·
IF 5.825
Jinfeng Han,Caixia Liu,Qingling Liu,Shuangchun Lu,Yalian Bi,Xiaohan Wang,Mingyu Guo,Chunfeng Song,Na Ji,Xuebin Lu,Degang Ma,Zhenguo Li
Novel Al-rich OFF-CHA twin-crystal zeolite was synthesized by one-pot hydrothermal method, and applied in ammonia-selective catalytic reduction (NH 3 -SCR) after copper ion exchange. Results indicated that Cu content in Cu-OFF-CHA played a significant role in NH 3 -SCR reaction. The insufficiency of copper activity sites and the formation of CuOx were the main reasons affecting low and high temperature SCR activity of catalyst, respectively. Cu 3.1 -OFF-CHA, with the optimal copper content, demonstrated over 90 % NOx conversion and exhibited excellent N 2 selectivity in the range from 160 to 550 ℃. Further research verified that the SCR activity of Cu 3.1 -OFF-CHA maintained above 80 % in the temperature range from 180–450 °C after hydrothermal treatment 16 h. The reason might be that Cu 2+ in Cu-OFF-CHA was migrated from CHA to OFF sites after hydrothermal treatment, and Cu 2+ in OFF sites on Cu-OFF-CHA was more stable, resulting in less conversion of the active site to CuOx clusters. Cu-OFF-CHA has the potential to be applied in SCR after-treatment systems of diesel exhaust due to the excellent SCR activity and hydrothermal stability.
研究领域:
催化化学
·
环境化学
·
材料科学
·
化学工程
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2018
·
IF 6.653
Yaxin Chen,Chao Li,Junxiao Chen,Xingfu Tang
Low-temperature selective catalytic reduction of NO by NH3 (NH3–SCR) is a promising technology for controlling NO emission from various industrial boilers, but it remains challenging because unavoidable deposition of ammonium bisulfates (ABS) in the stack gases containing both SO2 and H2O inevitably results in deactivation of catalysts. Here we developed a stable low-temperature NH3–SCR catalyst by supporting Fe2O3 cubes on surfaces of MoO3 nanobelts with NH4+-intercalatable interlayers, which enables Fe2O3/MoO3 to spontaneously prevent ABS from depositing on the surfaces. Using in situ synchrotron X-ray diffraction, 1H magic angle spinning nuclear magnetic resonance, and temperature-programmed decomposition procedure, the results demonstrate that NH4+ of ABS was initially intercalated in the interlayers of MoO3, leading to a NH4+-HSO4– cation–anion separation by conquering their strong electrostatic interactions, and subsequently the separated NH4+ was consumed by taking part in low-temperature NH3–SCR. Meanwhile, the surface HSO4– separated from ABS oxidized the reduced catalyst during the NH3–SCR redox cycle, concomitant with release of SO2 gas, thereby resulting in decomposition of ABS. This work assists the design of stable low-temperature NH3–SCR catalysts with strong resistance against deposition of ABS.
研究领域:
环境催化
·
材料科学
·
空气污染控制
·
无机化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.7
Weixiang Chen,Yuxiong Wang,Yaoyu Zhang,Yue Liu,Zhongbiao Wu
Ammonia (NH 3 ) has emerged as a promising zero‑carbon energy source for energy and transportation. However, its utilization leads to the emission of NH 3 , which contributes to PM 2.5 formation and disrupts the global nitrogen cycle. Selective catalytic oxidation (SCO) represents a mainstream technology for NH 3 treatment, yet achieving both sufficient activity and high N 2 selectivity across a broad temperature window remains challenging. Here, a core-shell Pt@Cu-ZSM-5 catalyst was employed for NH 3 catalytic abatement by encapsulating metallic Pt clusters (Pt 0 ) inside the channels of Cu ion-exchanged ZSM-5. The optimal sample achieved a complete NH 3 conversion below 250 °C and maintained over 92% N 2 selectivity from 250 to 500 °C due to the synergism between the Pt Cu dual sites. Mechanistic studies revealed that NH 3 oxidation preferentially occurred on Pt 0 sites with excellent redox capacity to produce N 2 O and NO x at relatively low and high temperatures, respectively. And the presence of Cu ions (Cu δ+ ) could efficiently both inhibit the formation of N 2 O on Pt 0 sites and reduce NO x emission, thereby improving the N 2 selectivity. At relatively low temperatures, NH 3 -solvated Cu + (NH 3 ) 2 could migrate to the adjacent Pt sites and reduce the adsorbed NO* species from NH 3 oxidation, damping the formation of N 2 O. At high temperatures, the NO and NO 2 emitted from Pt 0 sites could be reduced on Cu δ+ sites via a typical selective catalytic reduction. This study provides new insights into the rational design of bifunctional SCO catalysts and offers a comprehensive understanding of the synergistic effects in Pt Cu dual-site systems.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 21.1
Jie Yang,Yu Luo,Zhichao Chen,Junjiang Zhu
The selective catalytic reduction of NO with NH 3 (NH 3 −SCR) reaction is governed by the interplay of surface acidity and redox activity, yet the mechanism of their cooperation remains elusive. Herein, Ce–O–W linkages were constructed on Ce/ZrO 2 to couple Ce 4+ /Ce 3+ redox cycle with tungsten-derived acidity. Operando DRIFTS and transient experiments revealed that gaseous NO reacts directly with NH 3 adsorbed on Lewis Ce 4+ sites, following an Eley–Rideal pathway. Brønsted acid sites from Ce–O–W acted as NH 4 + reservoirs, dynamically replenishing Lewis-bound NH 3 and sustaining continuous reactivity. Operando UV–vis spectroscopy confirmed that NO + NH 3 exposure reduced Ce 4+ to Ce 3+ , while O 2 re-oxidized Ce 3+ to Ce 4+ , establishing the redox cycle. Density functional theory calculations supported that NH 3 dehydrogenation on Ce sites and subsequent coupling with gaseous NO were energetically favorable, while O 2 -assisted Ce 3+ re-oxidation required the highest energy barrier. These results highlight the cooperative function of Ce–O–W acid–redox site in promoting SCR activity through dynamic L–NH 3 /B–NH 4 + interplay and sustained Ce redox cycling.
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FUEL
·
2026
·
IF 7.5
Zhenhua Ji,Zhongqiang Bao,Zihao Wu,Peng Zhang,Rui Yang,Ding Luo,Hao Chen
As the most effective after-treatment technology for NH 3 emission control in road vehicles, Ammonia Slip Catalyst still faces challenges such as insufficient catalytic activity and low selectivity to the reaction product N 2 . Especially, the performance bottleneck in anti-aging greatly limits the commercial application of the catalyst, and there are still research gaps. Based on this, this study aims to reconstruct the structure − activity relationship of the catalyst by directionally constructing TiO 2 with a multi − scale channel core − shell structure as the support based on introducing different contents of Pt and Cu dual active components, and to explore the regulation and improvement mechanism of the catalytic performance including anti − aging property under the multi − dimensional synergistic effect. The results indicate that by enhancing the mass transfer capability of the catalyst with three-dimensional mass transfer channels and the influence of the dual active components, Pt 5 -Cu 1 /TiO 2 with a Pt − Cu content ratio of 5:1 achieves the best catalytic activity and N 2 selectivity. The Density Functional Theory calculation results show that due to the relatively low free energy of the key intermediate HNO, the Pt content plays a dominant role in the formation of N 2 O. Based on the relatively low free energy of the key intermediate NH 2 and the sequential dehydrogenation order, the thermodynamic conditions for the N 2 formation pathway under the catalytic action of Cu are extremely favorable, with relatively small kinetic barriers. Compared with Pt, the NO X formation pathway under the catalytic action of Cu has a smooth energy decrease and is more likely to occur, but it is also affected by the complex competition in the synergistic effect of the dual active components. The 17.69 % content of Pt 4+ in the active components of the catalyst after aging is the main reason for the decline in activity. The thicker shell layer reduces the collapse of the core–shell structure at high temperatures, laying a stable structure–activity relationship foundation for maintaining high activity. The prepared Pt 5 -Cu 1 /TiO 2 still meets the emission regulation limits after aging, showing good anti-aging performance.
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