Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Shoubing Chai,Yingjie Li,Wan Zhang,Zirui He
In carbonation stage of calcium looping process, NO could be reduced by CO using CaO as a catalyst, allowing simultaneous CO 2 and NO removal. However, to achieve efficient NO removal, the required CO/NO molar ratio in the carbonator is very high (up to 30:1), which leads to lots of unreacted CO in the exhaust gas. In this work, to maintain high efficiency of NO removal at low CO concentration in carbonator, Ce-doped CaO was employed to simultaneously enhance NO and CO 2 removal performance. The effects of Ce-doped CaO on simultaneous CO 2 and NO removal in bubbling fluidized bed reactor were investigated during the carbonation stage of calcium looping process. When the molar ratio of CO/NO is about 3.57:1, Ce-doped CaO obtains an 83% CO 2 capture efficiency and a 97% NO removal efficiency in 20 cycles in chemical reaction controlling stage. The average CO concentration in exhaust gas of Ce-CaO was reduced by 79% at the same NO removal efficiency as Mn-doped CaO. The presence of Ce 3+ makes the charge imbalance of the material, resulting in more charge transfer from the Ce-CaO surface to the molecules. The density functional theory reveals that Ce doping reduces the energy barriers of the conversion of NO to N 2 and the CO 2 adsorption, promoting the simultaneous NO/CO 2 removal in carbonation stage. Therefore, under a low molar ratio of CO/NO in carbonation stage of calcium looping, Ce considerably improves the simultaneous CO 2 and NO removal action of CO and CaO.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Qiuhui Zhu,Reshalaiti Hailili,Yue Xin,Yingtang Zhou,Yu Huang,Xinzhu Pang,Ke Zhang,Peter K.J. Robertson,Detlef W. Bahnemann,Chuanyi Wang
Developing full-spectrum responsive and efficient photocatalysts is still an important challenge in the field of photocatalytic treatment of trace environmental pollutants. Herein, full-spectrum Bi@Bi 2 Ti 2 O 7 with rich-oxygen vacancies (OVs) were fabricated via a one-pot hydrothermal method. The optimized composite photocatalyst exhibited a photocatalytic efficiency of 79 %, more than doubled higher than that of its counterpart, Bi 2 Ti 2 O 7 (31.79 %), for removing ppb-level NO under visible-near infrared (Vis-NIR) irradiation. The enhanced photocatalytic performance was attributed to the co-effect of Bi and OVs reveal by control experiments and theoretical calculations, which not only benefited the adsorption and photocatalytic activation of NO but broadened light absorption to near infrared region. Furthermore, the adsorption and photocatalytic conversion pathway of NO was explored by in situ DRIFTS, suggesting that NO + as intermediate species is crucial to improve the selectivity of NO converting to nitrate. This work provides a new perspective of constructing full-spectrum-driven photocatalysts for environment remediation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Shujun Sun,Jun Zhang,Changdong Sheng,Hui Zhong
A novel Na2SiO3/Fenton system was employed for NO removal from coal-fired flue gas in a bubble reactor. The NO removal efficiency of this system could reach 94.36% when the flue gas residence time was 3 s. The hydrolysis reaction of Na2SiO3 produced OH-, which made the solution alkaline, and the formation of iron-based colloids in the alkaline environment effectively catalyzed the generation of free radicals from H2O2, O2•– radicals, which was the main reason for the increase of NO removal efficiency. The reaction of H2O2 catalyzed by iron-based colloids increased the solution pH, which could not only further improve the NO removal efficiency but also enhance the useless decomposition of H2O2. Na2SiO3 could buffer the solution pH, which weakened the ineffective decomposition of H2O2 and prolonged the effective denitrification time. The X-ray diffraction and ion chromatography analysis showed that NO was finally converted to NO3– and NO2–.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Shujun Sun,Jun Zhang,Changdong Sheng,Hui Zhong
Currently, most advanced oxidation denitrification technologies require long flue gas residence time to obtain ideal NO removal efficiency. The NaOH-catalyzed H 2 O 2 system proposed in this paper can obtain 98% NO removal efficiency under the condition of flue gas residence time of 3 s. The mechanism of NO removal and H 2 O 2 decomposition to O 2 were proposed. It was confirmed with ESR (Electron-spin-resonance), inhibitor experiments and UV-Vis spectrophotometer that the main group in the reaction process was·O 2 - radicals, which reacted with NO to form ONOO - , and ONOO - would be gradually transformed into NO 3 - and NO 2 - in the air. The effect of some primary factors on the NO removal efficiency and the percentage of H 2 O 2 decomposition to O 2 were also investigated. The increase of initial pH has a positive effect on NO removal, while the promotion of NO removal by increasing H 2 O 2 concentration and reaction temperature is limited and the increase of NO has a negative effect on NO removal. Initial pH has a dual impact on the percentage of H 2 O 2 decomposition to O 2 , H 2 O 2 concentration and reaction temperature promote the decomposition of H 2 O 2 to O 2 , while NO concentration has an inhibiting effect on it.
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PubMed
高影响因子
Catalysts
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2022
·Vol. 12
·期 5
·534
·
IF 4.501
Zhaohui Teng,Shan Huang,Na Li,Qulan Zhou
Rice husk ash (RHA) has potential as a supporter of catalysts. In this research, we studied the activity and SO2tolerance of RHA-based Fe-Cu oxide in the reduction of NO by CO. Characterization methods were employed to study the properties of the catalysts and their SO2tolerance. Activity and SO2resistance were also tested at different temperatures. We recommend two catalysts with SO2resistance ability: Fe0.67Cu0.33/RHA (the highest catalytic activity) and Fe0.8Cu0.2/RHA. The NO removal rate hardly changed with the addition of SO2and was kept at about 100%. However, the CO conversion rate decreased with increasing SO2at the lower reaction temperatures, which may be due to the formation of sulfites. Fortunately, the deactivation was reversible and can be reduced with an increase in the reaction temperature. The results of our research may help promote the application of CO-SCR.Keywords:rice husk ash;Fe-Cu catalysts;NO reduction;SO2resistance;CO-SCR
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Materials Today Chemistry
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2022
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IF 7.613
T. Huang,Z. Yu,B. Yuan,L. Jiang,Y. Liu,X. Sun,P. Liu,W. Jiang,J. Tang
The presence of bacteria, existing as highly organized biofilm communities, in chronic non-healing wounds has been identified as a significant impediment for wound healing. Nanozymes , with unique antimicrobial mechanisms, as a new alternative for antibiotics, have the potential to synergize with nitric oxide (NO) with enhanced antibacterial and antibiofilm ability. However, the always-on state of nanozymes and the reactivity of NO limit their clinical applications. In this context, an intelligent and multifunctional Pd-MOF@PAzo@SNP nanoplatform was fabricated using UiO-66 as a palladium (Pd) nanozyme-loading vehicle, then a surface modification with photosensitive polyazobenzene (PAzo), and the adsorption of the NO donor sodium nitroprusside (SNP) via a host-guest interaction between β -cyclodextrin-modified hyaluronic acid ( β -CD-HA) and azobenzene. The activity of Pd-nanozyme was easily controlled via ultraviolet (UV) light, and its photosensitivity was regulated by changing the side-chain unit length of PAzo. Furthermore, NO was released in response to the UV irradiation and played a synergistic role with the peroxidase activity of Pd nanozyme, exhibiting excellent antibacterial and antibiofilm activity in the presence of 0.01 mM hydrogen peroxide (H 2 O 2 ). In vivo , Pd-MOF@PAzo@SNP accelerated the healing of a biofilm-infected diabetic wound by dispersing the biofilm, reducing bacterial burden, and promoting angiogenesis and collagen deposition. Overall, the nanoplatform provides a reliable and highly efficient strategy to develop an intelligent nanozyme synergy with NO therapy in chronic wound management.
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ADVANCED FUNCTIONAL MATERIALS
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2022
·Vol. 32
·期 41
·2205569
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IF 19.924
Chunpeng Bai,Shiying Fan,Xinyong Li,Zhaodong Niu,Jing Wang,Zhiyuan Liu,Dongke Zhang
Hollow nanoreactors show great potential in catalysis due to the void-confinement effect. Yet few studies have investigated the void-confinement effect of hollow nanoreactors on intermediates. Herein, electrochemical NO reduction to NH 3 (ENOR) is used as a probe reaction to study the void-confinement effect of hollow Cu 2 O@CoMn 2 O 4 nanoreactors on intermediates. Combined with the results of catalytic activity, H 2 -treated in situ diffusion Fourier transform infrared spectroscopy and the finite-element method simulation confirm that the void-confinement effect on the intermediate is the main reason for enhanced ENOR efficiency. Additionally, theoretical calculations also show that the Cu sites of Cu 2 O@CoMn 2 O 4 nanoreactors are favorable for the formation of *NOH intermediates. This work not only gives an insight into void-confinement effect of hollow nanoreactors on intermediates but also provides a valuable strategy for improving ENOR.
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Engineering
·
2023
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IF 12.8
Xiaoyu Li,Xiaoshu Lv,Jian Pan,Peng Chen,Huihui Peng,Yan Jiang,Haifeng Gong,Guangming Jiang,Li'an Hou
Photocatalysis offers a sustainable avenue for the oxidative removal of low concentrations of NO x from the atmosphere. Layered double hydroxides (LDHs) are promising candidate photocatalysts owing to their unique layered and tunable chemical structures, and the abundant hydroxide (OH − ) moieties on their surfaces that are hydroxyl radical ( • OH) precursors. However, inferior charge separation and limited active sites on an LDH hinder its practical applications. Herein, we developed a facile N 2 H 4 -driven etching (et) approach that introduces dual Ni 2+ and OH − vacancies (Ni v and OH v ) into NiFe-LDH nanosheets (referred to as NiFe-LDH-et) that facilitate improved charge-carrier separation and the formation of active Lewis acidic sites (Fe 3+ and Ni 2+ exposed at OH v ). In contrast to inert pristine LDH, NiFe-LDH-et actively removes NO when illuminated with visible light. Specifically, Ni 76 Fe 24 -LDH - et etched in 1.50 mmol·L −1 N 2 H 4 solution removes 32.8% of the NO from continuously flowing air (NO-feed concentration: ∼500 parts per billion (ppb)) when illuminated with visible light, thereby outperforming most reported catalysts. Experimental and theoretical data reveal that the dual vacancies promote the production of reactive oxygen species ( • O 2 − and • OH) and the adsorption of NO on the LDH. In-situ spectroscopy revealed that NO is preferentially adsorbed at Lewis acidic sites, particularly exposed Fe 3+ sites, and then converted into NO + that is subsequently oxidized to NO 3 − without the formation of any of the more toxic NO 2 intermediate, thereby alleviating risks associated with its production and emission.
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NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 43
·19974-19982
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IF 3.3
Hao Fan,Qin Peng,Zhenxing Shen,Xuefeng He,Yiming Yang
Nitric oxide (NO), a major atmospheric pollutant and a precursor to haze, can be removed using the denitration catalyst. Mn and Ni are commonly used as denitration catalyst additives owing to their adsorption abilities for NO and ammonia (NH3). In this study, we synthesized Mn- and Ni-loaded Pt-modified sulfated cerium oxide (PtSCe) catalysts using an impregnation method and explored the effects of these elements. The results revealed that the two elements had contrasting effects on the denitration activity of the catalysts. Mn improved the water vapor and sulfur resistance of the PtSCe sample by increasing the concentration of weak acid sites, enhancing the redox ability, and increasing the content of surface-adsorbed oxygen. The elevation in oxygen vacancies, stimulated by the presence of Ce3+ and Mn3+, swiftly replenished the reactive oxygen species, thereby sustaining the high denitration efficiency of the MnPt/SCe sample. Active sites on the catalyst surface included NH3 adsorbed on Lewis acid sites, NH4+, and –NH2, along with bridging, monodentate, and bidentate nitrate groups. Regarding the catalyst reaction mechanism, we determined that the selective catalyst reduction of NH3-SCR over MnPt/SCe followed both the Eley–Rideal and Langmuir–Hinshelwood mechanisms. These findings offer crucial insights into the intricate relationship between metals, sulfates, and carrier molecules, thus providing implications for future catalyst design.
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STARCH-STARKE
·
2021
·
IF 2.741
Meidong Li,Xiufang Huang,Qin Zhang,Yifeng Zhou,Kai Luo
Four new types of water-soluble polysaccharides are isolated from Cardamine hupingshanensis . Herein, this study examines C. hupingshanensis polysaccharide no. 2 (CHP-2) with a molecular weight of 21.75 kDa. Analysis revealed that CHP-2 is composed of d -glucuronic acid, d -galacturonic acid, glucose, galactose, and L-arabinose. It is speculated that the main connecting bond is →4)-α-D-Glc(p)-(1→), →t)-α-D-Glcp-(1→). Through perfusion experiments using streptozotocin-induced diabetic rats, oral CHP-2 solution is found to significantly reduce food intake, water intake, and fasting blood glucose levels, while increasing the weights of rats. In addition, CHP-2 significantly reduces the serum and liver malondialdehyde contents and increases the activity of the corresponding antioxidant enzymes. Moreover, the effect elicited by the CHP-2 solution is similar to that of phenformin hydrochloride solution. Hence, the results of this study suggest that CHP-2 exhibits blood sugar-lowering and anti-oxidation effects.
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ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 36
·2103949
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IF 18.808
Liangbin Xiong,Jiashuai Li,Feihong Ye,Haibing Wang,Yaxiong Guo,Xing Ming,Qingyun Chen,Shaoan Zhang,Ruihao Xie,Zhanxu Chen,Yang Lv,Guangqi Hu,Yingji He,Guojia Fang
SnO 2 compact layer (c-SnO 2 ) frequently suffers from degradation in high temperature processes (HTP) such as crack, worse interfacial contact, and electrical properties, that is, annealing effect. To solve this problem, a kind of bifunctional SnO 2 colloid is developed by using small molecular oxalate whose organic components can be removed clearly at a low temperature process (LTP). The c-SnO 2 and SnO 2 mesoporous layer (m-SnO 2 ) derived from the fresh and aged sols with the same colloid show no annealing effect, decreasing oxygen vacancy, and adsorbing water on increasing annealing temperature. The champion devices of LTP and HTP SnO 2 planar perovskite solar cells (PSCs) achieve, respectively, stabilized photoelectric conversion efficiencies (PCEs) of 20.74% and 20.70%. In contrast, the performance of champion devices of their mesoporous counterparts is significantly improved, showing nearly hysteresis free character with stabilized PCEs of 22.40% and 22.37%, respectively. The inclusion of m-SnO 2 plays a role of an energy bridge, improving electrons collection efficiency, which is supported by photoluminescence and transient photoluminescence characterizations. HTP SnO 2 mesoporous PSCs can preserve 97.6% and 80% of their initial PCEs after aging for 25 weeks and 8-h irradiated/16-h dark cycle within 104 h. The high stability of HTP SnO 2 PSCs may ascribe to low oxygen vacancy and adsorbed water of HTP SnO 2 .
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Guanyu Liu,Huiyun Xia,Yanhui Niu,Xu Zhao,Gengtong Zhang,Lifang Song,Huaxin Chen
Practical significance in terms of the long-term effective application of photocatalytic coatings is greatly challenged by its easy pollution and poor self-cleaning performance. In this paper, a self-cleaning photocatalytic WO 3 -TiO 2 nanorod (MWT) /PDMS building coating (MWT coating) was prepared by spraying methods. The surface hierarchical structure fabricated by MWT and PDMS was a crux to construct a superhydrophobic surface, which endowed MWT coating with self-cleaning performance. Besides, the MWT coating exhibited prominent durability and antifouling property after 450 d practical application of the external wall. The excellent self-cleaning property of the coating was confirmed by the removal and resistance to the adhesion of powder particles. Meanwhile, the photocatalytic properties of MWT endowed MWT coating with the ability to degrade organic pollutants on the surface. The color difference of the coating polluted by methyl red was only 1.18 and 4.77 after 24 h UV and visible irradiation, respectively. This mutual benefit effect of self-cleaning and photocatalysis was also reflected in the degradation of NO. In the first five cycles, the degradation efficiency of NO decreased by 4.74% gradually under visible light due to the adhesion of oxidation products, and most of the MWT on the coating surface was regenerated after flushing, the PCD efficiency increased by 3.71%. Furthermore, after 30 days of outdoor weathering test, the PCD efficiency of MWT coating decreased by 11.74% and 12.05% under UV and visible light, respectively, which lays a foundation for the long-term effectiveness of the MWT coating in the process of use.
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