Enhanced removal efficiency of multicomponent VOCs over the Sn-doped Silicalite-1-supported Ru single-atom catalysts by constructing tightly coupled redox and acidic sites - Details

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Abstract：

The　development　of　cost-effective　catalysts　with　excellent　chlorine　resistance　and　harmful　by-products　inhibition　is　important　for　the　environmentally　friendly　purification　of　multi-component　volatile　organic　compounds　(VOCs　and　chlorine-containing　VOCs　(CVOCs)).　In　this　work,　the　Sn-doped　Silicalite-1-supported　Ru　(Ru@Silicalite-1-Sn-x,　and　x　is　the　molar　ratio　of　Si/Sn)　samples　were　prepared　using　a　hydrothermal　strategy,　and　catalytic　activities　of　these　materials　were　investigated　for　the　oxidative　removal　of　mixed　VOCs　(dichloromethane　(DCM)　and　toluene).　The　Ru@Silicalite-1-Sn-50　sample　with　tightly　coupled　redox　and　acidic　sites　exhibited　high　catalytic　activity　(T90%　=　287　°C　for　toluene　oxidation　and　T90%　=　361　°C　for　DCM　oxidation　at　a　space　velocity　of　40,000　mL/(g　h);　specific　reaction　rate　and　turnover　frequency　(TOFRu)　for　toluene　oxidation　at　170　°C　were　9.67　μmol/(gcat　h)　and　0.98　×　10−3　s−1,　and　specific　reaction　rate　and　TOFRu　for　DCM　oxidation　at　200　°C　were　3.84　μmol/(gcat　h)　and　0.46　×　10−3　s−1,　respectively),　excellent　catalytic　stability　(within　100　h　of　on-stream　oxidation　at　380　°C),　and　effective　inhibition　of　toxic　chlorine-containing　by-products　formation　in　the　oxidation　of　(DCM　and　toluene).　The　doping　of　Sn　could　effectively　anchor　the　Ru　atoms　to　result　in　single-atom　dispersion　of　Ru　and　generate　oxygen　vacancies,　and　optimized　the　synergistic　interaction　between　Lewis　acid　sites　and　Brønsted　acid　sites.　The　high　concentration　of　oxygen　vacancies　and　enriched　Brønsted　acid　sites　promoted　the　cleavage　of　C−Cl　bonds　in　DCM　and　accelerated　the　desorption　of　Cl　species　as　inorganic　chlorine.　In　the　meanwhile,　the　strong　electron　transfer　within　the　Sn−O−Si　bond　increased　the　Lewis　acidity,　which　promoted　the　deep　oxidation　of　dechlorinated　intermediates/other　intermediates　over　Ru@Silicalite-1-Sn-50.　We　believe　that　the　present　work　provides　a　feasible　and　promising　strategy　for　the　design　of　efficient　catalysts　for　the　destruction　of　multicomponent　VOCs　and　CVOCs　in　an　industrial　scale.　©　2024　Elsevier　B.V.

Keyword：

Volatile organic compound Supported Ru single-atom catalyst Toluene Tin-doped Silicalite-1 Catalytic oxidation Dichloromethane

Author Community：

[ 1 ] [Wu L.]Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, China
[ 2 ] [Wu L.]Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 3 ] [Deng J.]Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, China
[ 4 ] [Deng J.]Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 5 ] [Liu Y.]Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, China
[ 6 ] [Liu Y.]Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 7 ] [Jing L.]Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, China
[ 8 ] [Jing L.]Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 9 ] [Yu X.]Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, China
[ 10 ] [Yu X.]Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 11 ] [Tao J.]Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, China
[ 12 ] [Tao J.]Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 13 ] [Gao R.]Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, China
[ 14 ] [Gao R.]Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 15 ] [Feng Y.]Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, China
[ 16 ] [Feng Y.]Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
[ 17 ] [Dai H.]Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, China
[ 18 ] [Dai H.]Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China

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