CARBON
·
2023
·
IF 10.9
Lizhen Hu,Jiayou Liu,Xiaoxiang Huang,Qianqian Nie,Penglei Liu,Zhongchao Tan,Hesheng Yu
Using nanoclusters and single atoms with unique activity to replace nanoparticles is a promising strategy to enhance catalyst activity. However, stable loading of nanoclusters and single atoms remain a challenge. This paper reports atomically dispersed Pt bridged with metal-organic framework (MOF)-derived ZnO/C through carbon atoms (Pt–ZnO/C), by impregnation combined with calcination , for photocatalytic oxidation of NO. The MOF-derived ZnO/C has a larger specific surface area than pure ZnO. The presence of C enhances the visible light absorption, promotes the migration of photogenerated carriers , and more importantly facilitates the stabilization of Pt single atoms through Pt–C interactions. The Pt species present in the Pt–ZnO/C catalysts in the form of single atoms and nanoclusters. The Pt–ZnO/C catalysts show high NO conversion rates and selectivity towards NO 3 − /NO 2 − ions formation. Specifically, the NO conversion rate of 81.9% is much higher than those of ZnO/C (31.4%) and Pt nanoparticles loaded ZnO/C (Pt NPs-ZnO/C, 58.6%). In addition, the selectivity of NO 3 − /NO 2 − (i.e., 98.6%) formation over the Pt–ZnO/C catalyst is much higher than that of NO 2 (i.e., 1.4%). Furthermore, the photocatalysis tests and ESR results suggest that the Pt single atoms and nanoclusters can enhance the oxidation of NO by promoting the production of O 2 •- and OH • . The DFT results also reveal that single Pt atoms promote the adsorption of O 2 and H 2 O to form O 2 •- and OH • . More importantly, OH • can promote the selective oxidation of NO to NO 3 − /NO 2 − ions. In addition, the projected density of states of single Pt atoms loaded on the ZnO/C catalysts show that the presence of C atom bridge favors the stability of single Pt atoms because of the interaction between C and Pt atoms. This work provides a new strategy for the design of single-atom-loaded metal oxide catalysts.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2014
·
IF 5.481
Yue Liu,Qingfeng Wang,Rongjun Mei,Haiqiang Wang,Xiaole Weng,Zhongbiao Wu
Recently, simultaneous removal of SO2, NOx and oxidized mercury in wet flue gas desulfurization (WFGD) scrubber has become a research focus. Mercury re-emission in traditional WFGD system has been widely reported due to the reduction of oxidized mercury by sulfite ions. However, in multipollutants simultaneous absorption system, the formation of a large quantity of nitrate and nitrite ions as NOx absorption might also affect the reduction of oxidized mercury in the aqueous absorbent. As such, this paper studied the effects of nitrate and nitrite ions on mercury re-emission and its related mechanism. Experimental results revealed that the nitrate ions had neglected effect on mercury re-emission while the nitrite ions could greatly change the mercury re-emission behaviors. The nitrite ions could initially improve the Hg0-emission through the decomposition of HgSO3NO2–, but with a further increase in the concentration, they would then inhibit the reduction of bivalent mercury owing to the formation of Hg-nitrite complex [Hg(NO2)x2-x]. In addition, the subsequent addition of Cl– could further suppress the Hg0 emission, where the formation of a stable Hg-SO3–NO2–Cl complex was assumed to be the main reason for such strong inhibition effect.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Na Zhou,Jiazhi Wang,Ning Zhang,Zhi Wang,Hengguo Wang,Gang Huang,Di Bao,Haixia Zhong,Xinbo Zhang
Electrochemical conversion of nitrate (NO 3 − ) pollutants into chemical feedstock and fuel ammonia (NH 3 ) can contribute to sustainable mitigation of the current severe energy and environmental crises. However, the electrocatalytic NO 3 − reduction to NH 3 (NRA) involves a sluggish multielectron and proton transfer process that competes with the hydrogen evolution reaction (HER) in aqueous media, imposing great challenges in developing highly selective catalysts for NRA. In this study, we developed a copper and copper-tetracyanoquinodimethane composite catalyst (Cu@CuTCNQ), which possesses a high density of copper vacancy defects. This catalyst has been proven to be efficient for NRA through an in situ electrochemical reconstruction method. The structural evolution of CuTCNQ during NRA was investigated by in situ Raman spectroscopy, which indicated an accelerated charge transfer from the CuTCNQ substrate to the derived Cu, which facilitated the adsorption activation of NO 3 − . The obtained Cu@CuTCNQ exhibited an excellent catalytic performance for NRA, with a Faradaic efficiency of 96.4% and productivity of 144.8 μmol h −1 cm −2 at −0.6 V vs . a reversible hydrogen electrode, superior to Cu nanoparticle counterparts and most Cu-based catalysts. Cu vacancy defects and sufficient interfacial charge transfer synergistically optimize the charge distribution of Cu active sites, reduce the energy barrier for NO 3 − adsorption, and promote deoxidation and hydrogenation processes, thus enhancing NRA and selectivity.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xun He,Long Hu,Lisi Xie,Zerong Li,Jie Chen,Xiuhong Li,Jun Li,Longcheng Zhang,Xiaodong Fang,Dongdong Zheng,Shengjun Sun,Jing Zhang,Abdulmohsen Ali Alshehri,Yongsong Luo,Qian Liu,Yan Wang,Xuping Sun
Nitrite (NO 2 − ), as a N -containing pollutant, widely exists in aqueous solution, causing a series of environmental and health problems. Electrocatalytic NO 2 − reduction is a promising and sustainable strategy to remove NO 2 − , meanwhile, producing high value-added ammonia (NH 3 ). But the NO 2 − reduction reaction (NO 2 − RR) involves complex 6-electron transfer process that requires high-efficiency electrocatalysts to accomplish NO 2 − -to-NH 3 conversion. Herein, we report NiS 2 nanoparticles decorated TiO 2 nanoribbon array on titanium mesh (NiS 2 @TiO 2 /TM) as a fantastic NO 2 − RR electrocatalyst for ambient NH 3 synthesis. When tested in NO 2 − -containing solution, NiS 2 @TiO 2 /TM achieves a satisfactory NH 3 yield of 591.9 µmol h −1 cm −2 and a high Faradaic efficiency of 92.1 %. Besides, it shows remarkable stability during 12-h electrolysis test.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemSusChem
·
2021
·Vol. 15
·期 4
·e202102049
·
IF 8.928
Pingping Huang,Tingting Fan,Xintao Ma,Jiguang Zhang,Yanping Zhang,Zhou Chen,Xiaodong Yi
Graphical Lowering barriers : Bimetallic ZnCo 2 O 4 catalyst can promote nitrate electroreduction at room temperature. The electron-deficient Co active site can lower the energy barriers for the formation of *NO 2 intermediate and suppress the hydrogen evolution reaction, thus enhancing the selectivity and yield rate of electrochemical NO 3 − reduction to ammonia. Nitrate (NO 3 − ) as a common pollutant of groundwater causes drinking water safety problems and seriously endangers people‘s health. Electrochemical reduction of nitrate to ammonia under ambient condition is a green and significant route to reduce the concentration of NO 3 − and produce ammonia (NH 3 ), known as a complement to the Haber–Bosch reaction. Currently, noble-metal electrocatalysts are often used in electrochemical reduction of NO 3 − , but high cost and scarcity limited their application. Herein, three-dimensional (3D) flower-like zinc cobaltite (ZnCo 2 O 4 ) electrocatalyst was developed to convert nitrate into ammonia at room temperature. The NH 3 yield rate could reach up to around 2100 μg mg −1 h −1 at a potential of −0.6 V vs. reversible hydrogen electrode (RHE), which was around 2.0 times higher than that of pristine Co 3 O 4 . In addition, the NH 3 faradaic efficiency of ZnCo 2 O 4 electrocatalyst could reach around 95.4 % at potential of −0.4 V vs. RHE with good structural and morphological stability, which surpassed most reported non-noble metal-based electrocatalysts. Further studies concluded that the improved activity of electrocatalytic NO 3 − reduction was ascribed to the existence of abundant active sites and the charge transfer from Co atoms to Zn atoms after Zn doping. Importantly, this work opens a new path for the development of Co-based materials as electrocatalysts for reducing nitrate to ammonia.
研究领域:
环境科学
·
电化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
You Xu,Kaili Ren,Tianlun Ren,Mingzhen Wang,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Electrochemical reduction of nitrate (NO 3 - ) to ammonia (NH 3 ) offers a sustainable avenue to close the NO 3 - cycle for NH 3 synthesis. Critical to the feasibility of electrochemical NO 3 - -to-NH 3 technology is the development of cost-effective, scalable and selective catalysts that can produce NH 3 with high yield. To this end, we design and constructure ultralow-content Pd (2.93 at%) in-situ incorporated Cu 2 O corner-etched octahedra (Pd-Cu 2 O CEO) with cavity and oxygen vacancy defects for selectively electrochemical NO 3 - -to-NH 3 transformation. The unique conner-etched cavity structure, rich surface oxygen vacancies, and Pd-Cu 2 O dual active sites, synergistically promote nitrate electroreduction undergo ammonia formation reaction pathway. Impressively, the as-made Pd-Cu 2 O CEO exhibited outstanding activity for electrocatalytic NO 3 - -to-NH 3 , with high ammonia selectivity (95.31%) and Faradaic efficiency (96.56%). The developed hierarchical-defect strategy may open a new avenue for reasonable design of defect electrocatalysts to contribute desirable properties and functionalities in specific applications.
研究领域:
电化学催化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Yajie Bai,Shuyu Gao,Wanru Xie,Zhenyuan Fang,Hongye Bai,Weiqiang Fan
Photoelectrochemical nitrate ions (NO 3 − ) reduction reaction (PEC NITRR) to produce ammonia (NH 3 ) at ambient conditions could not only solve the problem of NO 3 − pollution, but also transform the NO 3 − to hydrogen carrier (NH 3 ). Herein, we introduced Cu 2+ by construction of BiVO 4 /CuPc, effectively adsorbed target reactant NO 3 − and further promote its effective conversion to NH 3 . This unique catalyst structure leads to a desirable NH 3 yield (r NH3 = 12.98 μg h −1 cm −2 ) and Faraday efficiency (FE = 20.36%) at 0.1 V vs. RHE. Therefore, this work provides a new perspective for establishing a low energy consumption PEC NITRR to achieve sustainable transformation of pollutants.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Na Tong,Ying Wang,Yang Liu,Minbo Li,Zizhong Zhang,Huijuan Huang,Tao Sun,Jinxiang Yang,Fuying Li,Xuxu Wang
Photocatalytic ammonia synthesis is of great importance but remains very challenging in photocatalysis. Here, we fabricated a photocatalytic reaction system for the efficiently photocatalytic nitrate reduction to ammonia under UV irradiation using PdSn/NiO/NaTaO 3 :La as a photocatalyst in the presence of formic acid. Several important factors of the photocatalytic performance were investigated, including initial concentration of the nitrate solution, initial pH value and cocatalyst loadings. Nitrate conversion reaches 100% and ammonia selectivity is 72% over the optimum photocatalyst with 5% bimetallic PdSn alloy and 0.2% NiO loadings. The outstanding performance of photocatalyst can be ascribed to both the strong adsorption of nitrite on NiO and the efficient separation of electron-hole pairs by PdSn bimetallic alloy. Besides as the hole scavenger, formic acid also provides not only carboxyl anion radicals for nitrate reduction but also the in-situ buffer effect on ammonia formation. These results give inspiration for designing the reactive system with efficient photocatalytic ammonia synthesis.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Xihui Lu,Jinshan Wei,Hexing Lin,Yi Li,Ya-yun Li
Electrocatalytic reduction of nitrate (NO3RR) to ammonia offers a promising approach for mitigating the environmental impact of NO3–, while simultaneously enabling the synthesis of NH3 under ambient conditions. Recently, single-atom catalysts (SACs) have been proven to have attractive activity on NO3RR, and better catalysts with enhanced activity and stability are still in demand. Here, we report the efficient boosting of NH3 production via the NO3RR using boron-doped Fe SAC (Fe-BCN). Fe-BCN is a normal 12-hedral nanoparticle with a size of 500 nm. The NH3 Faradaic efficiency of Fe-BCN reached 97.48%, with a high ammonia production rate of 2.17 mg cm–2 h–1, in an alkaline electrolyte environment at an electrode potential of −0.3 V vs reversible hydrogen electrode. Density functional theory calculations revealed the strategy of introduced B regulating the intermediate adsorption on Fe-BCN, which enhanced the NO3RR activity. Furthermore, leveraging the high NO3RR activity of Fe-BCN, a nitrate-zinc battery with a power density of 0.90 mW cm–2 was constructed by using Fe-BCN as the cathode and zinc as the anode, respectively. This research demonstrates the broad prospects of Fe-BCN in the NO3RR and provides insights for high-performance Fe SAC electrode materials.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2024
·
IF 14.3
Jin Li,Qiuling Jiang,Xiujing Xing,Cuilian Sun,Ying Wang,Zhijian Wu,Wei Xiong,Hao Li
Electrochemical conversion of nitrate (NO 3 − ) to ammonia (NH 3 ) is a potential way to produce green NH 3 and remediate the nitrogen cycle. In this paper, an efficient catalyst of spherical CuO made by stacking small particles with oxygen-rich vacancies is reported. The NH 3 yield and Faraday efficiency are 15.53 mg h −1 mg cat −1 and 90.69%, respectively, in a neutral electrolyte at a voltage of -0.80 V (vs. reversible hydrogen electrode). The high activity of the electrodes results from changes in the phase and structure during electrochemical reduction. Structurally, there is a shift from a spherical structure with dense accumulation of small particles to a layered network structure with uniform distribution of small particles stacked on top of each other, thus exposing more active sites. Furthermore, in terms of phase, the electrode transitions from CuO to Cu/Cu(OH) 2 . Density functional theory calculations showed that Cu(OH) 2 formation enhances NO 3 - adsorption. Meanwhile, the Cu(OH) 2 can inhibit the competing hydrogen evolution reaction, while the formation of Cu (111) crystal surfaces facilitates the hydrogenation reaction. The synergistic effect between the two promotes the NO 3 - to NH 3 . Therefore, this study provides a new idea and direction for Cu-based oxides in electrocatalytic NH 3 production.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2019
·
IF 2.781
Min Yang,Yujia Yan,Huanxian Shi,Enzhou Liu,Xiaoyun Hu,Xu Zhang,Jun Fan
In this work, the fluorescent sensors based ternary ZnCdS quantum dots (QDs) were constructed for nitrite (NO 2 − ) detection, and ternary ZnCdS QDs were synthesized by a rather facile, low-cost and effective aqueous synthesis method using air-stable compounds. Experimental results indicated that the ZnCdS QDs fluorescence (PL) emission intensity was decreased gradually with the introduction of NO 2 − . Importantly, the F/F 0 (F and F 0 were the PL intensity in the presence and absence of NO 2 − at 505 nm, respectively) was linearly proportional to the NO 2 − to 700 μM, the equation of linear regression was y = −0.123x+1.1525, which showed a better performance to the detection of NO 2 − . Moreover, there was no interference to other interfering substances including metal ions and anion ions. Thus, we applied the ZnCdS QDs fluorescence sensors to detect the contents of NO 2 − in ham sausage and the results showed that the contents of NO 2 − in ham sausage was 18.45 mg/kg. Therefore, this test method had the advantages of simplicity, rapidity and high sensitivity.
研究领域:
分析化学
·
生物传感
·
食品科学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2023
·
IF 7.3
Ruixue Wang,Kun Li,Narcisse Tsona Tchinda,Wenxing Wang,Lin Du
Ammonia (NH3), the most common alkaline gas in the atmosphere, participates in heterogeneous reactions on the surface of aerosols and produces ammonium (NH4+). While most previous studies have focused on the effect of NH3 on the heterogeneous reactions of other gases on mineral dust aerosols, little research has been done on the heterogeneous reactions of NH3 influenced by acidic gases. Here, the effects of sulfur dioxide (SO2), formic acid, acetic acid and acrylic acid on the heterogeneous reaction of NH3 on the surface of nano α-Fe2O3 particles were investigated. We found that NH3 can promote the dissolution of α-Fe2O3 through NH3–Fe complexation and be oxidized to NO3−, while the addition of acidic gas inhibits the NH3–Fe complex formation and converts it into physical adsorption. SO2 promoted the conversion of NH3 to NH4+, while weakly inhibiting the oxidation of NH3 to NO3− by competing for oxidation sites under light conditions. Organic acids, on the other hand, inhibited the heterogeneous conversion of NH3, and strongly competed for oxidation sites under light conditions, significantly reducing NO3− production. This study reveals the various influences of acidic gases on NH3 heterogeneous reactions on α-Fe2O3 particles, which helps to improve the understanding of atmospheric processes involving NH3, acidic gases, and mineral dust aerosols.
研究领域:
大气化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）