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WASTE MANAGEMENT · 2023 · IF 8.1

Evolution and speciation transformation of chlorine during automobile shredder residue pyrolysis

Yang Ren,Hongyun Hu,Chengyang Cao,Guangzhao Guo,Xiaodong Zeng,Chan Zou,Xian Li,Hong Yao

Disposal of automobile shredder residue (ASR) via pyrolysis enables the recovery of valuable products; however, the production of hazardous pollutants and low-value products is inevitable due to its high chlorine content. In this work, chlorine evolution behavior and the conversion mechanism during ASR pyrolysis between 480 and 600 °C were systematically studied. The experimental results for organic chlorine (Org-Cl) showed that released chlorinated gases were complex, and HCl only accounted for 35% of the gas phase products, while short-chain hydrocarbons with carbon atoms between two and four accounted for 52%. Chlorine was predominantly retained in the char, and Org-Cl was the primary contributor to the residual chlorine, accounting for over 50% of the char. The content of inorganic chlorine (InO-Cl) was low in the raw sample but significantly increased in the char. Through the distinction between organic and inorganic chlorine content in char, it was confirmed that Org-Cl could be converted to InO-Cl due to complex secondary reactions with metallic compounds. The conversion was favored by increasing the Org-Cl content and the temperature. Our findings clarified the evolution mechanism of chlorine and the transformation from Org-Cl to InO-Cl, thus providing guidance for chlorine regulation and the efficient recycling of metal resources.

CAS / MDL: 9002-86-2
研究领域: 环境科学 · 化学工程
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Interstitial atom-doped NiFe alloy as pre-catalysts boost direct seawater oxygen evolution

Lumin Song,Dan Zhang,Hongfu Miao,Yue Shi,Mengna Wang,Liang Zhao,Tianrong Zhan,Jianping Lai,Lei Wang

NiFe-based materials are excellent OER electrocatalysts. However, it is difficult to stabilize anions and cations during reconstruction, which also leads to the problem of high valence metals at low levels and poor stability in direct seawater. Herein, we propose the strategy of using interstitial P atom-doped NiFe alloys (P 4.8 -NiFe ANs-400) as pre-catalysts to stabilize anions and cations, thereby promoting the formation of abundant high-valent metal species and excellent activity and stability in direct seawater. The reconstructed P 4.8 -NiFe ANs-400 catalyst generates a large amount of high-valence transition metal Ni 4+ , which contributed to its low overpotential (214 mV) and long-term stability (100 h) in a seawater electrolyte at 100 mA cm −2 . Experiments and theoretical calculations show that the interstitially doped P atoms share the charge around the Fe and the active Ni sites, optimizing the free energy of the OER intermediate and making the chlorine evolution reaction (CER) difficult to proceed.

研究领域: 材料科学 · 电化学 · 催化 · 可再生能源
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ELECTROCHIMICA ACTA · 2024 · IF 5.5

Flower-like NiCo2O4 spinel microspheres for efficient chlorine evolution under neutral conditions

Ran Zhang,Jing Cao,Ting Peng,KeXuan Wu,Yinqiang Shu

Dimensional stability anodes (DSA), constructed using noble metal oxides like RuO 2 and IrO 2 , is widely used in industrial chlorine production. The DSA electrode demonstrates exceptional chlorine evolution capabilities in acidic solutions and high-chloride concentrations. However, under neutral conditions, its chlorine evolution efficiency diminishes significantly. In this paper, a low-cost, high-efficiency 3D flower-like NiCo 2 O 4 catalyst was fabricated that exhibits high catalytic activity in neutral sodium chloride solutions. The 3D flower-like NiCo 2 O 4 catalyst exhibits good chlorine evolution efficiency, achieving 90 % at 30 mA/cm 2 in NaCl solutions. Furthermore, it's chlorine evolution efficiency of the electrocatalyst surpasses that of commercial DSA electrode at various current densities, making it a highly promising candidate for electrocatalytic applications.

CAS / MDL: 872-50-4
研究领域: 电化学 · 材料科学 · 催化
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ADVANCED MATERIALS · 2024 ·Vol. 36 ·期 31 ·2403792 · IF 27.4

Pt1.8Pd0.2CuGa Intermetallic Nanocatalysts with Enhanced Methanol Oxidation Performance for Efficient Hybrid Seawater Electrolysis

Kaiyang Xu,Lecheng Liang,Tong Li,Mujie Bao,Zhipeng Yu,Jingwei Wang,Sitaramanjaneya Mouli Thalluri,Fei Lin,Quanbing Liu,Zhiming Cui,Shuqin Song,Lifeng Liu

Seawater electrolysis is a potentially cost-effective approach to green hydrogen production, but it currently faces substantial challenges for its high energy consumption and the interference of chlorine evolution reaction (ClER). Replacing the energy-demanding oxygen evolution reaction with methanol oxidation reaction (MOR) represents a promising alternative, as MOR occurs at a significantly low anodic potential, which cannot only reduce the voltage needed for electrolysis but also completely circumvents ClER. To this end, developing high-performance MOR catalysts is a key. Herein, a novel quaternary Pt 1.8 Pd 0.2 CuGa/C intermetallic nanoparticle (i-NP) catalyst is reported, which shows a high mass activity (11.13 A mg PGM −1 ), a large specific activity (18.13 mA cm PGM −2 ), and outstanding stability toward alkaline MOR. Advanced characterization and density functional theory calculations reveal that the introduction of atomically distributed Pd in Pt 2 CuGa intermetallic markedly promotes the oxidation of key reaction intermediates by enriching electron concentration around Pt sites, resulting in weak adsorption of carbon-containing intermediates and favorable adsorption of synergistic OH − groups near Pd sites. MOR-assisted seawater electrolysis is demonstrated, which continuously operates under 1.23 V for 240 h in simulated seawater and 120 h in natural seawater without notable degradation.

研究领域: 材料科学 · 催化 · 电化学 · 可再生能源 · 纳米技术
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