JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Tiancheng Chu,Yong Zhang,Linghao Kong,Kuiling Li,Zhichao Zhao,Lili Xu,Xiaohui Wu,Jun Wang
Sulfide precipitation is a popular technique for the treatment and resource recovery of arsenic-containing dirty acid wastewater. However, this approach frequently suffers from toxic hydrogen sulfide (H 2 S) escape and agent wastage issues. Herein, a safe and efficient technique is proposed based on a polytetrafluoroethylene membrane contactor wherein the mass transfer resistance of the gas, membrane, and liquid phases can be easily and independently regulated to control the H 2 S supply. Additionally, H 2 S is transferred in bubble-free form, fundamentally avoiding the issue of gas escape, and uniform membrane distribution contributes to evenly distributed H 2 S delivery. The results demonstrated that 99.3 % arsenic precipitation could be achieved and the H 2 S emission ratio was limited to < 0.12 %, which was significantly better than traditional methods. Thus, highly efficient separation and resource recovery of heavy metals in wastewater can be achieved using this unique and controllable low-dose H 2 S supply method. The separation factor between copper and arsenic was as high as 7490.9. This study provides a safe, reliable, and promising new approach for the treatment of arsenic-containing acidic wastewater.
研究领域:
环境科学
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化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Ating Li,Hao Dong,Bo Wang,Shuangjiang Li,Tao Chen,Zhiyong Xu,Wenbo Zhao
To overcome high regeneration energy in conventional H 2 S capture processes, a novel non-aqueous solvent comprising sterically hindered tertiary-butylaminoethoxyethanol (TBEE) and triethylene glycol (TEG) was developed. At 30 wt% TBEE loading, exceptional H 2 S absorption capacity of 0.982 mol/mol was achieved under 0.6 bar and 293 K. Experimental characterizations combined with theoretical calculations analyses revealed that strong hydrogen-bonding networks between TBEE and TEG significantly enhanced thermal stability. Kinetic studies showed that the rate constants exhibited temperature- and pressure-dependent variations. Thermodynamic analysis using the Reaction Equilibrium Thermodynamic Model with physical absorption (RETM1-P) and van't Hoff equation obtained enthalpy (Δ H ) and entropy (Δ S ) values of −66.76 kJ/mol and −211.85 J/mol·K, respectively. Furthermore, the optimal absorption / desorption temperatures and theoretical desulfurization rate were determined. Moreover, the TBEE/TEG system show excellent recyclability with almost no significant decline in absorption capacity over ten consecutive absorption-desorption cycles, demonstrating its potential for long-term industrial application.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jianping Yang,Xingyue Zhou,Wei Zheng,Penglin Zhu,Fanyue Meng,Zequn Yang,Wenqi Qu,Hailong Li
Efficiently removing elemental mercury (Hg 0 ) from natural gas is a serious task to both equipment safety and ecosystem. The granulation of adsorbent powder is required to reduce pressure loss and adsorbent elutriation from a fixed-bed demercuration system. Herein, urea modified CuO (Urea/CuO) pellets were developed for Hg 0 adsorption from natural gas with H 2 S. The characterization results show that the addition of urea accelerated the formation of pore structure and surface oxygen, thus enhancing the Hg 0 adsorption performance of CuO pellets. The Urea/CuO pellets with 20 % urea additive amount exhibited 93 % Hg 0 removal efficiency under the existence of 500 ppm H 2 S and a gaseous hourly space velocity of 1.21 × 10 5 h −1 . H 2 S was essential to in-situ convert Urea/CuO pellets into a highly active Hg 0 adsorbent. With the increase of H 2 S concentration from 0 to 1000 ppm, the Hg 0 removal efficiency was raised from 34 % to 93 %. Urea/CuO pellets performed well for Hg 0 adsorption at 10–50 °C, which was the representative temperature window of natural gas processing. The Hg 0 adsorption capacity and uptake rate of Urea/CuO with 500 ppm H 2 S reached as high as 27.06 mg·g −1 and 2.44 μg·g −1 ·min −1 , which largely exceeded those of commercial activated carbons specialized for Hg 0 adsorption as well as typical granulated Hg 0 adsorbents reported in previous literature. The existence of H 2 S in natural gas in-situ converted CuO into CuS. The S 2 2− on the formed CuS could act as active sites for Hg 0 adsorption, in which gaseous Hg 0 was captured as stable mercury sulfide (HgS). The deactivated adsorbent could be regenerated and reused by thermally decomposing HgS and replenishing the consumed surface oxygen and the sintering surface. With these advantages, the developed Urea/CuO pellets appears to be a promising Hg 0 adsorbent from natural gas with H 2 S.
研究领域:
环境工程
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材料科学
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化学工程
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气体净化
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污染控制
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ACS Sensors
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2024
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IF 8.2
Huan Wang,Chonghui Zhu,Xiaohui Yan,Zhaorui Zhang,Huashuai Hu,Mengmeng Xu,Yu Liang,Minghui Yang
Fuel cell gas sensors have emerged as promising advanced sensing devices owing to their advantageous features of low power consumption and cost-effectiveness. However, commercially available Pt/C electrodes pose significant challenges in terms of stability and accurate detection of low concentrations of target gases. Here, we introduce an efficient Cu–Pt/CrN-based fuel cell gas sensor, designed specifically for the ultrasensitive detection of hydrogen sulfide (H2S) at room temperature. Compared to the commercial Pt/C sensor, the Cu–Pt/CrN sensor exhibits excellent sensitivity (0.26 μA/ppm), with an increase in the selectivity by a factor of 2.5, and demonstrates good stability over a 2 month period. The enhanced sensing performance can be attributed to the modulation of the electronic arrangement of Pt by Cu, resulting in an augmentation of H2S adsorption. The Cu–Pt/CrN fuel cell gas sensor provides an opportunity for detecting parts per billion-level H2S in various applications.
研究领域:
材料科学
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传感器技术
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环境监测
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Green Energy & Environment
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2024
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IF 10.7
Xu Liu,Liang Shan,Xiaoxue Sun,Tianxin Wang,Zhongqing Liu,Yuefeng Liu
Removing hydrogen sulfide (H 2 S) via the selective oxidation has been considered an effective way to further purify the indusial sulfur-containing due to it can completely transform residual H 2 S into elemental sulfur. While N-doped porous carbon was applied to H 2 S selective oxidation, a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty, limiting its future development in large-scale applications. Herein, we present porous, honeycomb-like N-doped carbon catalysts with large specific surface areas, high pyridinic N content, and numerous structural defects for H 2 S selective oxidation prepared using reusable NaCl as the template. The as-prepared NC-10-800 catalyst exhibits excellent catalytic performance (sulfur formation rate of 784 g sulfur kg cat. −1 h −1 ), outstanding stability (> 100 h), and excellent anti-water vapor, anti-CO 2 and anti-oxidation properties, suggesting significant potential for practical industrial application. The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity. Importantly, the water-soluble NaCl template could be easily washed from the carbon nanomaterials, and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors. This environment-friendly, low-cost, reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.
研究领域:
材料科学
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环境工程
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TALANTA
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2026
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IF 6.7
Xinru Chang,Song Guo,Xia Zhou,Zhendong Tang,Shuai Chen
Semiconductor metal oxides (SMOs) are widely used in gas sensing and detection due to their low cost, ease of manufacture, and portability. However, single SMO for hydrogen sulfide (H 2 S) detection suffers from high operating temperatures, low sensitivity, and poor selectivity. This study focused on designing multifaceted SMO materials, and three-dimensional openwork structure YMn 1-x Fe x O 3 composites were prepared using the premixed stagnation flame method. The prepared gas sensor showed high sensitivity to H 2 S gas. Specifically, the YMn 0.7 Fe 0.3 O 3 sensor has a maximum response value of 10.55 at an optimum operating temperature of 200 °C when exposed to 30 ppm H 2 S. It also demonstrated a low detection limit of 0.94 ppm and excellent selectivity, which is advantageous for long-term practical applications. The excellent sensing performance is attributed to the three-dimensional openwork structure of the material and the successful doping of Fe 3+ into the YMnO 3 lattice. These features increase the specific surface area, which facilitates the diffusion and adsorption of H 2 S gas in the sensing layer. The YMn 1-x Fe x O 3 materials provide a viable strategy for designing highly responsive and selective SMO gas sensors for detecting H 2 S.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Shiyan Li,Hongquan Fu,Xingshuai Zhang,Xu Liu,Giulia Tuci,Giuliano Giambastiani,Cuong Pham-Huu,Yuefeng Liu
H 2 S selective oxidation to elemental sulfur (S 8 ) is a typical reaction where the mass product diffusion ( e.g ., S 8 ) through the catalytic bed is crucial as well as the reagents accessibility ( e.g ., H 2 S, O 2 ) to the active sites. The NaNO 3 -assisted pyrolysis of polyacrylamide was applied to synthesize defect-enriched N-doped carbon nanosheets with thickness up to c.a. 2 nm, featured by fully accessible and highly interconnected pores, for boosting the H 2 S selective oxidation process. The PAM-0.3-700 sample has revealed an unprecedented desulfurization activity with sulfur formation rate of 1165 g sulfur kg cat. −1 h −1 , other than a remarkable stability (>80 h). Experimental and theoretical studies have unveiled the critical role of edge sites containing unpaired electrons and nitrogen species with respect to the material aptitude towards O 2 dissociation and HS - activation. The material in presence of a highly interconnected porous network facilitates the reactants/product diffusion especially for catalysis operated under harsh experimental conditions.
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ENERGY & FUELS
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2017
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IF 3.091
Kuan Huang,Jia-Yin Zhang,Xing-Bang Hu,You-Ting Wu
The development of ionic liquid-based absorbents for selective separation of H2S from CO2 is of interest to the natural gas industry. In this work, a series of tertiary-amine functionalized protic ionic liquids (TA-PILs) were synthesized by neutralizing one of the tertiary amine groups in diamine compounds with acetic acid, leaving the other tertiary amine group as the functional site for selective absorption of H2S. To overcome the high viscosity of pure ionic liquids, TA-PILs were dissolved in water to give mixed absorbents. The effects of TA-PIL species, TA-PIL concentration, and experimental temperature on the solubilities of H2S and CO2, and absorption kinetics of H2S and CO2 in aqueous TA-PILs were investigated systematically. The reaction equilibrium constants and absorption enthalpy of H2S and CO2 in aqueous TA-PILs were also calculated by correlating the solubility data with a reaction equilibrium thermodynamic model. Results demonstrated that aqueous TA-PILs have high absorption capacities for H2S. Although the equilibrium selectivities of H2S/CO2 in aqueous TA-PILs are minimized, they still display significant kinetic selectivities for the two gases. More importantly, the TA-PILs designed are featured with low cost and facile synthesis, making them more attractive than other functionalized ionic liquids reported in the literature for application in selective separation of H2S from CO2.
研究领域:
化学工程
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环境科学
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MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Yu Zhou,Hui Gong,Hou-Jing Liu
Efficient, selective and highly sensitive detection of H 2 S is important for environmental protection and human security. Nanomaterials-based cataluminescence (CTL) sensors, especially metal-free catalysts, have been used for gas sensing. Herein, due to the efficient electron transfer and high specific area of silicon nitride (Si 3 N 4 ), combined with the strong electronegativity of fluorine and oxygen, we purposely synthesized F and O-modified Si 3 N 4 (F/O-Si 3 N 4 ) by engineering surface states and catalytic properties. We then used it to construct a H 2 S CTL gas sensor. Compared with other metal-based CTL sensors, the F/O-Si 3 N 4 -based CTL system exhibited high sensitivity and a longer lifetime stability. The detection limit was 0.027 μg mL −1 in the detection range of 0.49–8.17 μg mL −1 , and a relative standard deviation (RSD) of better than 3.3% were obtained. Further research demonstrated the luminescence mechanism, in which the rich oxygen vacancies of Si 3 N 4 promoted the adsorption of O 2 and the formation of F-Si sites due to the catalytic oxidation of H 2 S and the generation of SO 2 *. This served as the main emitter accounting for the strong CTL emission. This work is the first report of the application of Si 3 N 4 as a catalyst for CTL H 2 S sensing. This will expand the methods for enhancing the catalytic activity and practical applications of metal-free materials.
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JOURNAL OF CONTROLLED RELEASE
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2023
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IF 10.8
Yuzhi Qiu,Man Fan,Yiqian Wang,Xiuwen Hu,Jiawen Chen,Samir Kamel,Yajiang Yang,Xiangliang Yang,Hongfang Liu,Yanhong Zhu,Qin Wang
The continuous supply of hydrogen sulfide (H 2 S) gas at high concentrations to tumors is considered a promising and safe strategy for tumor therapy. However, the absence of a durable and cost-effective H 2 S-producing donor hampers its extensive application. Sulfate-reducing bacteria (SRB) can serve as an excellent H 2 S factory due to their ability to metabolize sulfate into H 2 S. Herein, a novel injectable chondroitin sulfate (ChS) hydrogel loaded with SRB ( [email protected] Gel) is proposed to sustainably produce H 2 S in tumor tissues to overcome the limitations of current H 2 S gas therapy. In vitro , the ChS Gel not only supports the growth of encapsulated SRB, but also supplies a sulfate source to the SRB to produce high concentrations of H 2 S for at least 7 days, resulting in mitochondrial damage and immunogenic cell death . Once injected into tumor tissue, the [email protected] Gel can constantly produce H 2 S for >5 days, significantly inhibiting tumor growth. Furthermore, such treatment activates systemic anti-tumor immune responses, suppresses the growth of distant and recurrent tumors , as well as lung metastases , meanwhile with negligible side effects. Therefore, the injectable [email protected] Gel, as a safe and long-term, self-sustained H 2 S-generating factory, provides a promising strategy for anti-tumor therapy.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Chengjiu Zhao,Xuezheng Guo,Yanqiao Ding,Chengyao Liang,Bingsheng Du,Wen Niu,Weijie Qu,Yijie Shi,Shuren Cong,Gang Meng,Yong He
Complex gas environments and the demand for room temperature detection will provide challenges for chemo-resistive-type gas sensors in a variety of applications. In this work, 2D/0D SnSe 2 /TiO 2 composite is used as a sensing material, displaying good sensitivity and specificity to ppb-level NO 2 at ambient temperature (25 °C). The response value and time of the SnSe 2 /TiO 2 sensor are 207 % and 139s when exposed to 100 ppb NO 2 , as opposed to 62 % and 183s for the pristine SnSe 2 sensor. The composite sensor also offers great long-term stability for NO 2 and good gas selectivity. Notably, the SnSe 2 /TiO 2 sensor's mixed gases (NO 2 +H 2 S) measurement is done to examine its NO 2 detection capacity in the presence of interfering gas. The constructed composite sensor can accurately detect NO 2 even if the concentration of the reductive interfering H 2 S is 66.7 times higher than that of the oxidative target NO 2 . The effective usage of SnSe 2 modified by TiO 2 for low-concentration, room-temperature NO 2 detection in a complex gas environment is shown by the composite sensor's pleasing gas detection results.
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INORGANICA CHIMICA ACTA
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2023
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IF 2.8
Zheng Li,Jing Wang,Xiaoxia Peng,Yu Chen,Mengyuan Geng
Hydrogen sulfide plays an essential roles in physiological and pathophysiological process. It is still a challenge to design a simple and reasonable H 2 S-specfic fluorescent probe. Herein, we develop a simple reaction-based fluorescent probe for detecting H 2 S in DMF/Tris-HCl buffer system. Fluorescence emission spectra were used to investigate the recognition performance of probe L towards hydrogen sulfide. The results shown that probe L has a specific recognition towards hydrogen sulfide over other tested metal cations and anions with a rapid response. The probe L combined with H 2 S in a 1: 1 manner with a detection limit of 0.372 μM. The appropriate pH range for detecting H 2 S was 4 ∼ 8. The proposed recognition mechanism was studied by fluorescence titration spectrum, Job’s plot, 1 H NMR titration experiment and mass spectrometry analysis. Moreover, probe L was applied in real water samples, test strips and fluorescent films to detect H 2 S successfully.
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