增效Zr掺杂的3d打印NiZr0.1/SiOC整体催化剂增强低温CO2甲烷化：双途径机理和结构稳定性

IF 7.7 2区工程技术 Q1 CHEMISTRY, APPLIED

Fuel Processing Technology Pub Date : 2025-09-08 DOI:10.1016/j.fuproc.2025.108328

Honglei Mi , Yifan Zhang , Faliang Luo

{"title":"增效Zr掺杂的3d打印NiZr0.1/SiOC整体催化剂增强低温CO2甲烷化：双途径机理和结构稳定性","authors":"Honglei Mi , Yifan Zhang , Faliang Luo","doi":"10.1016/j.fuproc.2025.108328","DOIUrl":null,"url":null,"abstract":"<div><div>Monolithic Ni<img>Zr<sub>0.1</sub>/SiOC catalysts with tailored architectures were fabricated via direct ink writing (DIW) 3D printing for CO<sub>2</sub> methanation. Zr doping markedly enhanced low-temperature activity (<300 °C) by improving Ni dispersion, strengthening metal-support interactions, and suppressing particle agglomeration. Structural characterization revealed that Zr doping optimized pore accessibility and active-site exposure, while in situ studies confirmed a dual-pathway reaction mechanism involving formate and CO intermediates. The 30 % Ni<img>Zr<sub>0.1</sub>/SiOC catalyst exhibited exceptional performance, achieving 95.09 % CO<sub>2</sub> conversion at 320 °C and 91.56 % at 290 °C with 100 % CH<sub>4</sub> selectivity. Long-term stability tests (335 h) demonstrated robust anti-coking and anti-sintering properties, attributed to Zr-induced stabilization of Ni nanoparticles. This work highlights the synergy between additive manufacturing and dopant engineering for designing high-performance catalysts for CO<sub>2</sub> methanation.</div></div>","PeriodicalId":326,"journal":{"name":"Fuel Processing Technology","volume":"278 ","pages":"Article 108328"},"PeriodicalIF":7.7000,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"3D-printed NiZr0.1/SiOC monolithic catalysts with synergistic Zr doping for enhanced low-temperature CO2 methanation: dual-pathway mechanism and structural stability\",\"authors\":\"Honglei Mi , Yifan Zhang , Faliang Luo\",\"doi\":\"10.1016/j.fuproc.2025.108328\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Monolithic Ni<img>Zr<sub>0.1</sub>/SiOC catalysts with tailored architectures were fabricated via direct ink writing (DIW) 3D printing for CO<sub>2</sub> methanation. Zr doping markedly enhanced low-temperature activity (<300 °C) by improving Ni dispersion, strengthening metal-support interactions, and suppressing particle agglomeration. Structural characterization revealed that Zr doping optimized pore accessibility and active-site exposure, while in situ studies confirmed a dual-pathway reaction mechanism involving formate and CO intermediates. The 30 % Ni<img>Zr<sub>0.1</sub>/SiOC catalyst exhibited exceptional performance, achieving 95.09 % CO<sub>2</sub> conversion at 320 °C and 91.56 % at 290 °C with 100 % CH<sub>4</sub> selectivity. Long-term stability tests (335 h) demonstrated robust anti-coking and anti-sintering properties, attributed to Zr-induced stabilization of Ni nanoparticles. This work highlights the synergy between additive manufacturing and dopant engineering for designing high-performance catalysts for CO<sub>2</sub> methanation.</div></div>\",\"PeriodicalId\":326,\"journal\":{\"name\":\"Fuel Processing Technology\",\"volume\":\"278 \",\"pages\":\"Article 108328\"},\"PeriodicalIF\":7.7000,\"publicationDate\":\"2025-09-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fuel Processing Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0378382025001523\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fuel Processing Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0378382025001523","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}

引用次数: 0

摘要

采用直接墨水写入（DIW） 3D打印技术制备了具有定制结构的单片NiZr0.1/SiOC催化剂，用于二氧化碳甲烷化。Zr掺杂通过改善Ni分散、加强金属支撑相互作用和抑制颗粒团聚，显著提高了低温活性（<300°C）。结构表征表明，Zr掺杂优化了孔隙可达性和活性位点暴露，而原位研究证实了涉及甲酸酯和CO中间体的双途径反应机制。30% NiZr0.1/SiOC催化剂表现出优异的性能，在320°C和290°C下，CO2转化率分别达到95.09%和91.56%，CH4选择性为100%。长期稳定性测试（335小时）显示出强大的抗焦化和抗烧结性能，这归功于锆诱导的Ni纳米颗粒的稳定。这项工作强调了增材制造和掺杂工程之间的协同作用，以设计高性能的二氧化碳甲烷化催化剂。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

查看原文本刊更多论文

3D-printed NiZr0.1/SiOC monolithic catalysts with synergistic Zr doping for enhanced low-temperature CO2 methanation: dual-pathway mechanism and structural stability

Monolithic NiZr_0.1/SiOC catalysts with tailored architectures were fabricated via direct ink writing (DIW) 3D printing for CO₂ methanation. Zr doping markedly enhanced low-temperature activity (<300 °C) by improving Ni dispersion, strengthening metal-support interactions, and suppressing particle agglomeration. Structural characterization revealed that Zr doping optimized pore accessibility and active-site exposure, while in situ studies confirmed a dual-pathway reaction mechanism involving formate and CO intermediates. The 30 % NiZr_0.1/SiOC catalyst exhibited exceptional performance, achieving 95.09 % CO₂ conversion at 320 °C and 91.56 % at 290 °C with 100 % CH₄ selectivity. Long-term stability tests (335 h) demonstrated robust anti-coking and anti-sintering properties, attributed to Zr-induced stabilization of Ni nanoparticles. This work highlights the synergy between additive manufacturing and dopant engineering for designing high-performance catalysts for CO₂ methanation.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

Fuel Processing Technology 工程技术-工程：化工

CiteScore

13.20

自引率

9.30%

发文量

398

审稿时长

26 days

期刊介绍： Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.