Journal of Environmental Chemical Engineering
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2026
·Vol. 14
·期 5
·124092
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IF 7.5
Zhihui Li,Xiangyu Wang,Hua Jiang,Kexin Zhu,Zihan Li,Fuping Zeng
To address the environmental challenge of sulfur hexafluoride (SF 6 ), a CuO@ZnO catalyst was prepared from a Cu/Zn-BTC bimetallic precursor. This enabled a synergistic treatment system with sulfur element-catalyzed conversion and fluorine element-fixation. The experimental results show that under mild conditions of 500 °C and 0.2 MPa, during a 20 h catalytic process, the catalyst achieves a maximum degradation efficiency of 96.34% for 2% SF 6 , with high selectivity converting it to SO 2 , while fluorine was fixed as CaF 2 . In-situ XRD characterization and density functional theory (DFT) calculations revealed a key in situ activation process. Under NH 3 induction, CuO is reduced to metallic Cu, forming an optimal Cu@ZnO interface that enhances SF 6 adsorption and bonding. This significantly lowers the energy barriers for S-F bond cleavage and SO 2 formation. The rate-determining step, the energy barrier for SO 2 formation, dropped from 2.74 eV to 0.48 eV compared with CuO@ZnO, thus providing a kinetic explanation for the catalytic mechanism. Overall, this work offers a high-performance catalyst for SF 6 treatment and a new theoretical basis for designing MOF-derived materials for fluorinated greenhouse gas conversion.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Dan Baohui,Mahmood ul Haq,Salah Ud Din,Shabab Hussain,Shao Wenyi,Wu Jingmin,Chi Hanwen,Zhizhen Ye,Liping Zhu
The SF 6 gas in gas-insulated switchgear (GIS) systems decomposes into SO 2 F 2 , SOF 2 , SO 2 , and H 2 S under abnormal conditions such as partial discharge. The detection of these decomposition gases with high sensitivity is essential for the safe operation of GIS devices. Herein, we report the synthesis of cerium oxide and multiwalled carbon nanotube composite (CeO 2 @MWCNTs). The CeO 2 @MWCNTs composite was characterized by X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy , X-ray photoelectron spectroscopy, and Brunauer–Emmett–Teller analysis. The CeO 2 @MWCNTs composite sensor provided a response value of 7.7 at 100 ppm of SO 2 F 2 at a low operating temperature (50 °C), and the response and recovery features of the CeO 2 @MWCNTs composite sensor were recorded at 43 and 28 s, respectively. Moreover, the composite sensor exhibited excellent stability after two months. The developed CeO 2 @MWCNTs composite sensor can offer an exceptional platform for gas sensing applications in diverse fields.
研究领域:
材料科学
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气体传感技术
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电力设备监测
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纳米复合材料
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环境监测
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Li Jinjian,Chen Yuting,Ke Tian,Jin Yuanyuan,Fan Rongrong,Xu Guihong,Yang Liu,Zhang Zhiguo,Bao Zongbi,Ren Qilong,Yang Qiwei
Physisorption presents a promising alternative to cryogenic distillation for capturing the most potent greenhouse gas, SF 6 , but existing adsorbents face challenges in meeting diverse chemical and engineering concerns. Herein, with insights into in-pore chemistry and industrial process design, we report a systematic investigation that constructed two low-cost composites pellets (Al(fum)@2%HPC and Al(fum)@5%Kaolin) coupled with an innovative two-stage Vacuum Temperature Swing Adsorption (VTSA) process for the ultra-efficient recovery of low-concentration SF 6 from N 2 . Record-high selectivities (> 2×10 4 ) and SF 6 dynamic capacities (~ 2.7 mmol/g) were achieved, while exceptional SF 6 productivities (~ 58.7 L/kg), yields (~ 96.8%), and recyclability (~ 1000 cycles) were demonstrated in fixed-bed adsorption-desorption experiments under mild regeneration conditions. 2D solid-state NMR/in-situ FTIR, DFT-D binding/diffusion simulation analyses revealed the multi-site binding mode and the ultra-fast diffusion of SF 6 within the channels. The proposed VTSA processes successfully met the dual stringent requirements of both environmental protection and electricity equipment operation: the SF 6 recovery of 99.91% accompanied with a SF 6 purity/working capacity of 99.91%/2.1 mmol/g, which significantly outperformed the industrial employed adsorbent zeolite 13X and showed only 18.7% the energy consumption of the cryogenic distillation.
研究领域:
材料科学
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环境工程
·
化学工程
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Ziqi Si,Boxu Dong,Shan Zhu,Yue Zhao,Wenhui Zhou,Xinhua He,Fengxiang Ma,Jiantao Zai,Xuefeng Qian
Sulfur hexafluoride (SF 6 ) is a potent greenhouse gas widely used in electrical insulation due to its exceptional dielectric properties. Existing technologies are hampered by intractable issues such as prohibitive energy consumption and catalyst fluorination, making continuous operation difficult. Herein, we present a novel strategy leveraging synergistic Brønsted acid–oxygen vacancy (V o ) sites on a phosphoric-acid modified CeO 2 catalyst (PCe-90). This unique bifunctional design retains intrinsic V o of CeO 2 while introducing dense P–OH acid sites via a simple surface modification. Under 365 nm LED irradiation PCe-90 delivers 4.27 mL g −1 SF 6 mineralization within 24 h (8.5× pristine CeO 2 ). Crucially, PCe-90 demonstrates exceptional long-term robustness, maintaining undiminished activity over six cycles and 96 h of continuous operation without structural degradation. Mechanistically, P–OH protonates and polarizes the inert S–F bond, while V o injects electrons into the σ*(S–F) orbital to enable complete scission. This work establishes a synergistic catalytic mechanism and delivers a scalable, energy-efficient, and durable solution for practical SF 6 emission abatement.
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Catalysts
·
2026
·Vol. 16
·期 8
·696
·
IF 4.5
Zhenhua Cai,Kexin Zhu,Dongwei Sun,Zhihui Li,Xiangyu Wang,Zihan Li,Hua Jiang,Fuping Zeng
Sulfur hexafluoride (SF6) serves as an essential insulating and arc-extinguishing medium in power facilities, while it is an extremely potent greenhouse gas with an ultra-long atmospheric lifetime. To realize efficient medium-temperature harmless disposal of waste SF6, two-dimensional stable C4N monolayers were adopted as substrates to load ZnO and CuO nanoparticles for composite catalyst fabrication. XRD, TEM, and EDS characterizations confirmed the uniform dispersion of the metal oxides without destroying the C4N two-dimensional skeleton. Comparative experiments proved that an NH3reducing atmosphere significantly accelerates SF6decomposition. The 3:1 CuO-modified catalyst achieved a maximum SF6conversion of 91%, and a CaO additive effectively restrained high-temperature sintering and irreversible HF halogen poisoning, boosting overall catalytic efficiency by approximately 30%. DFT adsorption simulations revealed totally different active centers: hollow sites dominate ZnO-C4N with broad adsorption capacity for SO2, SO2F2, and other fluorinated intermediates, whereas surface O sites of CuO-C4N exhibit exclusive strong chemisorption toward SO2. Combined with macroscopic kinetics and atomic-scale interfacial interaction rules, their distinct stepwise defluorination pathways were illustrated. This study offers solid experimental data and microscopic theoretical guidance for designing advanced C4N-based catalysts for waste SF6abatement.
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ACS Applied Polymer Materials
·
2026
·Vol. 8
·期 14
·12068-12079
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IF 5.2
Chen Tao,Li Shuangjiang,Wang Bo,Yang Zhen,Xu Zhiyong,Zhao Wenbo
A highly potent greenhouse gas, sulfur hexafluoride (SF 6 ), requires efficient capture from industrial SF 6 /N 2 mixtures. Herein, a series of benzene-rich hyper-cross-linked
polymers (PPBx) were synthesized via a low-cost Friedel–Crafts
alkylation reaction using α,α ′ -dichloro- p -xylene (DCX) and triphenylbenzene (TPB) at different molar
ratios. The abundant benzene rings in the material enable strong F–π
interactions with SF 6 , while the hierarchical micromesoporous
structure ensures high adsorption capacity. Adsorption tests revealed
that PPB1, fabricated at a DCX/TPB molar ratio of 3:1, achieved a
remarkably high SF 6 uptake of 2.05 mmol/g at 298 K and
1 bar and an impressive SF 6 /N 2 ideal adsorbed
solution theory selectivity of 120 at 298 K. In addition, the dynamic
separation performance for SF 6 /N 2 was up to
1274.6 s/g, also demonstrating excellent properties under actual operating
conditions. The PPB1 material also demonstrates excellent thermal
stability and cycling performance. This work provides a cost-effective
and highly efficient hyper-cross-linked polymeric adsorbent with high
potential for industrial SF 6 separation and recovery.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Ating Li,Shuangjiang Li,Bo Wang,Tan Li,Wenbo Zhao,Honghong Liu,Zhiyong Xu
Constructing porous carbon adsorbents with SF 6 -matched ultramicropores is an effective route for recovering SF 6 from nitrogen-rich gas streams. Herein, hemin was introduced into ZIF-8 precursors to regulate pyrolysis-induced pore evolution and produce Fe,N-containing porous carbons without corrosive KOH activation. The optimized Fe,N-C-1000 displayed a large BET surface area of 1772.60 m 2 ·g −1 along with abundant ultramicropores mainly distributed at 0.5–0.65 nm, providing suitable confined spaces for adsorption of SF 6 . The Fe,N-C-1000 delivered an SF 6 adsorption capacity of 4.58 mmol·g −1 and an IAST selectivity of 222 at 298 K and 1.0 bar. Fixed-bed breakthrough tests verified the preferential retention of SF 6 over N 2 , as well as good regenerability and cycling stability. Structure-performance analysis suggests that the improved separation performance is mainly governed by hemin-directed ultramicropore formation, while the Fe/N-containing surface environment contributes additionally to SF 6 affinity. DFT calculations further support stronger SF 6 interaction with the Fe,N-C model than with the undoped carbon model. These results demonstrate that hemin-assisted pyrolysis provides a feasible KOH-free strategy for constructing MOF-derived ultramicroporous carbons for the capture and recovery of SF 6 .
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Runze Dong,Wenhao Li,Qiyu Yang,Ping Li,Pan Zhang,Lemeng Wang,Dong Fu
How to achieve low energy consumption and high degradation efficiency (DRE) under mild conditions is an important issue in the field of sulfur hexafluoride (SF 6 ) treatment. In this work, a new route of SF 6 degradation promoted by Ni-doped ceria (NiO-CeO 2 ) in a packed bed dielectric barrier discharge (PB-DBD) was proposed. The effects of Ni/Ce molar ratio, input power, SF 6 concentration and flow rate on the DRE of SF 6 were investigated. Compared with DBD or CeO 2 -DBD alone, the combination of DBD and NiO-CeO 2 can significantly promote the SF 6 degradation at lower input power. The Experimental results show that when the dosage of catalyst 1.5NiO-CeO 2 (Ni/Ce mole ratio is 1.5%) is 5 g, DBD input power is 50 W and SF 6 (1.5% SF 6 /98.5% Ar) flow rate is 100 ml·min −1 , the highest DRE can reach 97.7% and the energy yield can reach 11.5 gSF 6 ·(kWh) −1 . Adjusting the catalyst dosage according to the flux of SF 6 ( e.g., using 10 g catalyst to degrade SF 6 with a concentration of 1.5% and a flow rate of 80 ml·min -1 ), the DRE of nearly 99% can be achieved for a long time, which is crucial for industrial application. The mechanism deduction shows that the rich surface and mesopores of the catalyst are beneficial to the adsorption of SF 6 and intermediates, while the doping of Ni can significantly increase the content of oxygen vacancies to improve the degradation. Meanwhile, when NiO-CeO 2 is activated by DBD, the free O· can further promote the degradation. It is this coupling effect that leads to the high efficiency and low energy consumption of SF 6 degradation under mild conditions. It can be expected that this coupling technology route will have a good application prospect in the field of SF 6 treatment.
研究领域:
环境科学
·
材料科学
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SENSORS AND ACTUATORS B-CHEMICAL
·
2026
·
IF 8.3
Faxun Wang,Junyi Lin,Yuxuan Huang,Jiguang Zhao,Bing Tian,Liang Zhao,Bofeng Luo,Zhenliang Ye,Hao Yang,Guotao Duan
Reliable, drift-resistant monitoring of SF 6 enrichment in air near gas-insulated switchgear (GIS) leak points remains challenging for compact and low-cost sensing nodes. Here we report a thermal-conductivity-differential sensor enabled by a materials-circuit co-design: a hierarchical AlN@h-BN/MWCNT nanocomposite coating is integrated onto a Pt-coil element and read out by a Wheatstone bridge with a sealed reference arm and differential amplification. The ternary architecture exhibits a well-developed mesoporous framework with a high BET surface area (111.03 m 2 ·g −1 ), promoting efficient gas transport within the sensing layer and strengthening the thermal-conductivity-induced perturbation of the bridge balance. Under synthetic dry air (21% O 2 /79% N 2 ) at 25 ± 1℃, the output is monotonic over 0.1–5.0% SF 6 , with a recommended linear regime of 0.1–1.0% for quantitative readout; the baseline noise (σ air = 0.16 mV) yields an estimated LOD (3σ) of 0.0654% (∼654 ppm), while 0.1% is the lowest experimentally validated concentration. The optimized excitation voltage (3.0 V) maximizes response by balancing gas-phase modulation against increased non-gaseous heat losses at higher temperatures. The sensor shows reversible cycling (52/23 s response/recovery), humidity-tolerant operation (± 8% deviation over 20–80% RH), and < 5% degradation over 90 days; as expected for a TCD-type mechanism, cross-responses are governed by thermal conductivity rather than chemical selectivity.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Meng He,Xin Zhu,Yehui Ding,Lianjun Wang,Yuxing Luo,Xiangdong Ding,Xue Liu
Sulfur hexafluoride (SF 6 ) is a widely used insulating gas and a greenhouse gas which requires efficient recycling to minimize its environmental impact. Conventional membrane materials, such as zeolites, polymers, and metal-organic frameworks (MOFs), often suffer from harsh fabrication conditions or insufficient selectivity/permeability. In this work, we present a facile strategy for fabricating a noncovalently bonded polyaromatic hydrocarbon (PAH) monolayer membrane for efficient N 2 /SF 6 separation. The PAH monolayer with a thickness of 1.35 nm was prepared via Langmuir Schaefer (LS) method by using hexa(terpyridine) hexaphenylbenzene (HTPHPB) on air-water interface. Strong π-π stacking interaction between HTPHPB molecules stabilizes the monolayer, while the resulting intermolecular transient nanopores enable selective SF₆ separation from N₂. The resulting 4 layers of HTPHPB membrane, assembled at 25 mN·m −1 , exhibits exceptional SF 6 /N 2 separation performance with a selectivity of 155 ± 4 and a N 2 permeance of 136 ± 4 GPU, overcoming the inherent trade-off between selectivity and permeability in traditional organic membranes. Notably, the membrane maintains its separation performance even under bending, demonstrating excellent mechanical flexibility. This study offers a tunable and scalable organic membrane design strategy, paving the way for industrial applications in SF 6 recovery and gas separation.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2026
·
IF 4
Runze Dong,Dakuo Liu,Pengfei Qu,Wenhao Li,Dong Fu
This study proposes a novel approach for synergistically degrading sulfur hexafluoride (SF 6 ) using dielectric barrier discharge (DBD) combined with TiO₂/CeO₂ photocatalysis. By introducing UV-responsive TiO₂, the photocatalytic activity of the catalyst was significantly enhanced, thereby improving the overall degradation performance for SF 6 . Under the conditions of a Ti/Ce molar ratio of 0.05:0.95 and an input power of 60 W, a degradation efficiency (DRE) of 99.99% was achieved when degrading 2% SF₆. Compared with pure CeO 2 (with a DRE of 92.44%), the DRE has increased by 7.55%, and the selectivity of SO 2 in the product has also significantly improved, indicating that the doping of TiO 2 promotes the more complete degradation of SF 6 . Compared to using DBD alone, the DRE increased by 4.7 times, and the energy yield (EY) increased by 12.78 g/kWh. Density functional theory (DFT) calculations indicate that the TiO₂/CeO₂ composite catalyst enhances the surface adsorption capacity for SF 6 molecules. Mechanistic analysis further revealed that the UV light generated by DBD excites TiO₂/CeO₂ to produce photogenerated electron-hole pairs, while the high-energy electrons in the plasma region effectively suppress carrier recombination. This study confirms the significant potential of the DBD-photocatalysis synergistic system for treating highly stable SF 6 .
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