ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Bo Zhang,Jing Bai,Yan Zhang,Changhui Zhou,Pengbo Wang,Lina Zha,Jinhua Li,Abdolreza Simchi,Baoxue Zhou
H2S and CO2 are the main impurities in raw natural gas, which needs to be purified before use. However, the comprehensive utilization of H2S and CO2 has been ignored. Herein, we proposed a fully resource-based method to convert toxic gas H2S and greenhouse gas CO2 synchronously into CO and elemental S by using a novel electrochemical reactor. The special designs include that, in the anodic chamber, H2S was oxidized rapidly to S based on the I–/I3– cyclic redox system to avoid anode passivation. On the other hand, in the cathodic chamber, CO2 was rapidly and selectively reduced to CO based on a porous carbon gas diffusion electrode (GDE) modified with polytetrafluoroethylene and cobalt phthalocyanine (CoPc). A high Faraday efficiency (>95%) toward CO was achieved due to the enhanced mass transfer of CO2 on the GDE and the presence of the selective CoPc catalyst. The maximum energy efficiency of the system was more than 72.41% with a current density of over 50 mA/cm2, which was 12.5 times higher than what was previously reported on the H2S treatment system. The yields of S and CO were 24.94 mg·cm–2·h–1 and 19.93 mL·cm–2·h–1, respectively. A model analysis determined that the operation cost of the synchronous utilization of H2S and CO2 method was slightly lower than that of the single utilization of H2S in the existing natural gas purification technology. Overall, this paper provides efficient and simultaneous conversion of H2S and CO2 into S and CO.
研究领域:
环境科学
·
能源化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 25
·13798-13805
·
IF 2.936
Lianghu Su,Chenwei Liu,Kangkang Liang,Yudong Chen,Longjiang Zhang,Xiaolin Li,Zhihua Han,Guangyin Zhen,Xiaoli Chai,Xu Sun
The removal performance of high-concentration H2S (ca. 10 000 ppm) from simulated biogas by zero-valent iron nanoparticles (NZVI), with the majority of the particles in the size range of 60–150 nm, at different reaction temperatures (room temperature, 100 °C, 200 °C and 250 °C) were evaluated using a custom-designed quartz fixed-bed reactor. The results showed that the H2S removal capacities of NZVI were quite limited at room temperature and 100 °C, being 12.56 and 14.77 mg H2S gNZVI−1, respectively. However, these values increased significantly to 391.02 (200 °C) and 488.95 (250 °C) mg H2S gNZVI−1. Scanning electron microscopy analysis showed that the products of the NZVI–H2S reaction aggregated to form irregular polygonal-shaped structures. The main X-ray diffraction pattern peaks of the product matched well with troilite, and no pyrite was observed. The deconvolution of the X-ray photoelectron spectrometry peaks showed the presence of monosulphide (S2−) and disulphide (S22−) in the product, in which 36% of the sulphur existed as monosulphide and 64% as disulphide. It is proposed that the effective removal of hydrogen sulphide by NZVI at elevated temperatures can be attributed to the combination of nano-constituents, oxide shell and underlying Fe core to produce FeS similar to troilite and amorphous FeS2.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Haifeng Li,Sheng Su,Yan Peng,Linkang Wu,Kai Xu,Lijun Liu,Mengxia Qing,Song Hu,Yi Wang,Jun Xiang
High temperature sorbents for removing H2S comprising manganese oxide and Al2O3 support modified with La loadings were prepared with wet impregnation. The removal of H2S and the regeneration of sorbents were conducted at 850 °C to investigate the effect of the support modified with La on the desulfurization ability and durability of the Mn/La/Al2O3 sorbents. The fresh sorbent, first sulfide sorbent, and fourth regenerated sorbent were characterized by nitrogen isothermal adsorption, X-ray power diffraction, scanning electron microscopy, and H2 temperature-programmed reduction. The results showed that the highest initial breakthrough sulfur capacity (BSC) was obtained with Mn/0.78%La/Al2O3(M/0.78L), and the initial BSC decreased with increased La loadings due to the inhibiting of excessive La on the reaction between MnO and H2S. The BSC of sorbents with lower La loadings suffered more serious deactivation than MnxOy/Al2O3 during successive desulfurization–regeneration cycles, and the BSC durability of sorbents increased with an increase in La loadings and calcination temperature of La/Al2O3. Mn/4.83%La/Al2O3 with La/Al2O3 calcined at 900 °C (M/4.83H) had the best BSC durability, which was better than the BSC durability of MnxOy/Al2O3 (M) during several desulfurization–regeneration cycles. The characterization results showed that the structure of the M/4.83H sorbent was more stable than other sorbents. The M/4.83H sorbent derived the La(AlO3) phase, which could maintain the structural stability of the sorbent during several desulfurization–regeneration cycles. The formation of the LaAlO3 phase may inhibit MnxOy from dissolving into Al2O3, which was beneficial for the durability of sorbents during several successive desulfurization–regeneration cycles.
研究领域:
化学工程
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Sheng Huang,Husheng Shan,Yafei Xu,Jia Zuo,Yulong Zhao,Xiuquan Gu
Metal-halide perovskite (MHP) nanocrystals (NCs) have unique advantages in the gas sensing field, but the poor stability restricts their widespread applications. In this work, the CsPbBr 3 @Fe 2 O 3 heterojunction NCs were synthesized successfully by simple solution process and subsequent surface modification strategy for constructing a gas sensor. The Fe 2 O 3 shell layer was obtained through thermal decomposition of acetylacetone iron (AAI) at 400 °C. The resulting CsPbBr 3 @Fe 2 O 3 heterostructured NCs exhibit a higher gas-sensing performance to H 2 S than pure CsPbBr 3 and Fe 2 O 3 , respectively. Upon exposure to 10 ppm H 2 S, the response value of 4.12 was obtained at a moderate working temperature of 350 °C, while the response was fast both in terms of response time and recovery time, i.e. , 1.84 s and 24.20 s, respectively. This might be the best performance for MHP sensors, to the best of our knowledge. The excellent gas-sensitive response might be attributed to the formation of a heterojunction which promotes the electron migration from CsPbBr 3 to Fe 2 O 3 .
研究领域:
材料科学
·
纳米技术
·
气体传感
·
化学传感器
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS RESEARCH BULLETIN
·
2023
·
IF 5.4
Zhen Zhao,Lei Zhang,Hongming Zhang,Wuhong Xin,Xiaowen Wang,Chunmiao Liu,Yang Guo,Yinghua Zhuang,Wanli Jiao
Investigating high-performance and low-energy consumption H 2 S sensors has become a hot research topic. This study adopted a one-step co-precipitation method to synthesize La-doped ZIF-8 deprotonating zinc acetate, lanthanum nitrate, and 2-Methylimidazole in an aqueous. La 2 O 3 /ZnO were synthesized with different La 3+ doping concentrations (0, 0.5, 1, and 1.5 at%). We found that La 3+ doping at a concentration of 1 at% showed the highest response value of 140 for 5 ppm H 2 S, at a low operating temperature of 100 °C, which is 2.4 times higher than that of pure ZnO. Additionally, La 3+ doping led to a lower detection limit of 1.9 ppb. The enhanced performance can be attributed to the widening of the difference in electron concentration, the increase in vacant oxygen content, and the spillover effect of H 2 S sensing. These factors were analyzed in detail by means of porosity, P-N heterojunctions, and the increased in adsorbed oxygen content caused by La 3+ doping.
研究领域:
材料科学
·
传感器技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Weigang Chen,Chonghui Zhu,Mengmeng Xu,Xichao Mo,Minghui Yang
Hydrogen sulfide (H2S) monitoring is essential due to its toxicity and importance as a signaling molecule. Here, we introduce a Pt nanoparticle-loaded Mo0.33W0.67N sensor engineered for trace H2S detection featuring nanoparticle clusters with a 10–50 nm pore structure. It demonstrates exceptional selectivity and sensitivity, reaching 0.21 μA/ppm with a detection limit as low as 50 ppb, and maintains robust stability over 3 months. Notably, it outperforms commercial Pt/C electrodes with enhanced sensing capabilities attributed to the unique properties of ternary metal nitrides. By integrating the advantages of binary nitrides with multivalent cations and a specialized crystal structure, the Mo0.33W0.67N substrate achieves strong Pt interactions and improved sensor performance. This study highlights the potential of ternary metal nitride-based sensors for high-precision long-term H2S monitoring in environmental applications.
研究领域:
材料科学
·
电化学
·
环境监测
·
传感器技术
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2024
·
IF 5.6
Yan Su,Pengfei Gao,Guomei Zhang,Ying Zhou,Lihong Shi,Jianlin Wu,Wenting Liang,Shaomin Shuang,Yan Zhang
In this study, the N-Acetyl- l -Cysteine (NAC)-capped gold and silver bimetallic nanoclusters (NAC@Au–Ag NCs) was synthesized by reflux method. Due to the silver effect, the NAC@Au–Ag NCs exhibited strong photoluminescence at far-red/near-infrared regions and better catalytic performance than Au or Ag NCs. Upon addition of H 2 S, the Au–Ag NCs exhibited obvious fluorescence quench and color changes through the generation of metal sulfides and a static quenching process. The Au–Ag NCs displayed a wide linear luminescence response for H 2 S (18.5–217 μmol/L) with a detection limit of 0.269 μmol/L. Moreover, the visible color of Au–Ag NCs changed from white to brown-yellow along with increased H 2 S, the corresponding RGB values also displayed good linearity with the concentration of H 2 S (90.1–678 μmol/L). Notably, the fabrication of test strips provided a convenient and intuitive tool to screen the freshness of eggs by the color change of test strips. Au–Ag NCs could be used for living HeLa cells bioimaging and recognition of H 2 S abnormalities. Furthermore, it can be used as a catalyst to reduction of nitrophenols (NPhs), specific included 2NP, 3NP and 4NP. The reaction was regarded as a pseudo-first-order kinetic reaction due to the presence of excess NaBH 4 . At 298K, the catalytic rate constants(k) of 2NP, 3NP and 4NP were 0.1754 min −1 , 0.1734 min −1 and 0.2782 min −1 , respectively. The NAC@Au–Ag NCs catalyst still showed good catalytic activity and reusability after five cycles. Therefore, this study developed a H 2 S sensor for food samples and biological systems. And this nanocatalyst had great application potential for removed the nitrophenol pollutants in water.
研究领域:
分析化学
·
生物医学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2021
·
IF 6.609
Haifeng Li,Tao Liu,Sheng Su,Mei Jin,Wen Fang,Lijun Liu,Yi Wang,Song Hu,Jun Xiang
Ce modified Mn x O y /Al 2 O 3 -La have been prepared to investigate the effect of Ce loadings on pre-breakthrough H 2 S removal efficiency, breakthrough sulfur capacity (BSC) and BSC durability of the sorbents during desulfurization-regeneration cycles. The results showed Ce modification could improve the pre-breakthrough H 2 S removal efficiency of regenerated sorbents during desulfurization-regeneration cycles. The XPS characterization showed that the Ce can promote the binding energy of Mn ion to shift to lower energy, which enhanced H 2 S adsorption on the regenerated sorbent. However, the Ce loading sequence had effect on BSC durability of sorbent during desulfurization-regeneration cycles. The Ce-Mn x O y /Al 2 O 3 -La with co-impregnation of Mn and Ce oxides had higher BSC than Mn x O y /Al 2 O 3 -La, while the Ce/Mn x O y /Al 2 O 3 -La with Ce loading on the surface of Mn x O y /Al 2 O 3 -La had lower BSC and worse BSC durability than Mn x O y /Al 2 O 3 -La. The characterization results showed Ce-Mn x O y /Al 2 O 3 -La obtained better surface area and pore structure than Mn x O y /Al 2 O 3 -La, and Ce ion can promote the increasing of the around electron density of Mn ion, which was beneficial for H 2 S adsorption of Ce-Mn x O y /Al 2 O 3 -La. The poor surface area and pore structure would cause the low BSC of Ce/Mn x O y /Al 2 O 3 -La, and less stability of pore structure might lead to poorer BSC durability of Ce/Mn x O y /Al 2 O 3 -La than Mn x O y /Al 2 O 3 -La during desulfurization-regeneration cycles.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lin Chen,Xia Jiang,Shenggui Ma,Wenhua Chen,Bo Xu,Zhongde Dai,Wenju Jiang,Yue Peng,Junhua Li
In this study, Edge-N-rich carbon nanosheet @ porous biochar (NCN@PB) was synthesized successfully from waste biomass self-assembly in a simple and green approach. The accessible and efficient utilization of edge-N enriched on the surface, together with the hybrid structure of NCN@PB improved the H 2 S oxidation capacity up to 390.1 mg/g at room temperature, reflecting an 8-fold enhancement compared with the blank biochar. The Density functional theory calculation, in-situ DRIFTS, and the characterization results further uncovered the desulfurization mechanism of active sites. Edge-N species decreased the barriers in critical steps governing H 2 S catalytic oxidation, i.e., H 2 S dissociation and O 2 activation, especially the pyrrolic N. This strategy is beneficial for the development of surface engineering on metal-free catalysts and provides a new idea for improving the catalytic combustion activity of N-doped biochar.
研究领域:
环境科学
·
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Jiaxi Hu,Hongjie Song,Cheng Chen,Lichun Zhang,Mingxia Sun,Yi Lv
Cataluminescence as a highly efficient gas transduction principle has attracted wide attention among research in environmental monitoring and clinical diagnosis with increasing awareness of human safety. Nowadays, the development of innovation sensing systems and the construction of the sensing mechanism to improve the analytical performance of compounds remain a major challenge. Herein, we construct an advanced photoinduced thermocatalytic chemiluminescence (PI-TC-CL) gas-sensing system via the introduction of a Z-scheme heterojunction Ag3PO4/Ag/Bi4Ti3O12 to achieve higher efficient detection of H2S. The unique electron transport path of the Z-scheme heterojunction and the LSPR effect of Ag nanoparticles fascinate the generation of the photoinduced electron–hole pair on the surface of catalysts when stimulated by LED lamps and slow down the recombination of electron–hole pairs under thermal conditions. Thus, based on the cooperative effect of the Z-scheme heterojunction AgPO/Ag/BTO and PI-TC-CL system, we have successfully established an efficient H2S CTL detection system, which has a response three times higher than that on the traditional CTL system and even 45 times higher than that on BTO and ranges among the best of the state-of-the-art CTL performance in H2S detection with the linear range of 0.095–8.87 μg mL–1 and a limit of detection of 0.0065 μg mL–1. Besides, to explore the gas-sensing mechanism, the synergetic effects of photoinduction and thermal catalysis are investigated thoroughly via conductivity and electrochemical experiments. This research provides a new perspective of engineering highly efficient catalysts and ingenious sensor systems through designing the nanostructure of materials and synergism catalytic mechanism.
研究领域:
环境科学
·
分析化学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Feng Zhu,Xingyun Hu,Linghao Kong,Xianjia Peng
Sulfide precipitation is an efficient method to remove Cu(II) and As(III) from strongly acidic wastewater, but the instantaneous release of H 2 S from traditional sulfuration reagents causes serious H 2 S pollution. Moreover, the obtained precipitates are mixtures of CuS and As 2 S 3 , leading to difficulties in resource recovery. In this study, a calcium sulfide-organosilicon complex (CaS-OSCS), in which CaS was coated into a matrix of {[O 1.5 Si(CH 2 ) 3 NH]CS} n (OSCS) via the coordination bonding, was developed. OSCS, as a matrix of CaS-OSCS, can ensure the sustained and stable release of H 2 S under strongly acidic conditions owing to its low swelling (1.75% swelling ratio) and excellent acid resistance. The release longevity of H 2 S from CaS-OSCS extended from 5 min up to 50 min compared with that from CaS because the hydrophobic OSCS prevented solution diffusing to the pores of CaS-OSCS and thus slowed down the hydrolysis of CaS in pores. 99% of Cu(II)/As(III) was precipitated without H 2 S escape, and the dosage of sulfuration reagents was reduced by 30%. In addition, CaS-OSCS improved the selective separation of copper from wastewater, and a separation factor between Cu(II) and As(III) reached 2376. This study provides a potential approach for the elimination of H 2 S pollution and selective recovery of copper.
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
WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 7
·1-13
·
IF 2.9
Chen Sheng nan,Gao Ying jun,Ming Hao,Ren Long long,Geng Cong,Shen Xin jun,Shen Chen guang,Guan Yin yan,Gao Wei chun
Non-thermal plasma (NTP) co-catalytic technology is a waste gas treatment technology with high energy efficiency and little by-product. Catalyst plays an important role in the process of NTP co-catalytic degradation of contaminants. However, the performance of the catalyst is not only directly related to active center but also closely related to carrier. In this study, we successfully prepared stable Cu-doped catalysts with bicontinuous structure, using Cu(NO 3 ) 2 , Al(NO 3 ) 3 , and tetramethoxysilane as precursors through sol–gel process accompanied by phase separation. Scanning electron microscopy (SEM), energy dispersion X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), temperature programmed desorption (TPD), Brunauer–Emmett–Teller method (BET), and mercury intrusion porosity (MIP) were used to investigate the structure, properties, and the role of Al. It was found that in this Cu-doped system, addition of Al can produce Brønsted acidic sites and facilitate the divalent Cu dope into neutral Si skeleton to form stable complexes. Then, it was used as catalyst in NTP system to study the performance of the system and degradation mechanism of H 2 S. When binary metal catalyst was used, synergistic NTP system creates a secondary electron emission to enhance the field strength, 20 mg·m −3 H 2 S has the best degradation efficiency, and Cu-doped catalysts can cyclic utilization. At the same time, selective oxidation occurs in the system; elemental sulfur is produced.
研究领域:
环境科学
·
催化材料
·
等离子体技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）