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学者利用载氧体构建新策略实现甲烷高效制烯烃—新闻—科学网
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color: #333333; font-family: 宋体; line-height: 20px"> <b></b></td> </tr> </table> <p> </p> <p style=";; margin: 0px 0px 26px; text-align: justify; word-break: break-all;"> 近日，中国科学院广州能源研究所废弃物处理与资源化利用研究室副研究员赵坤，联合美国北卡罗莱纳州立大学、华东理工大学、美国里海大学等研究团队，利用载氧体构建新策略实现甲烷高效制烯烃。相关成果发表于《自然-通讯》。</p> <p style=";; margin: 0px 0px 26px; text-align: justify; word-break: break-all;"> 该研究报道了一种在以碳酸锂（Li<sub>2</sub>CO<sub>3</sub>）修饰的具有氧化还原活性的复合稀土金属氧化物催化作用下，实现低温高效化学链甲烷氧化偶联制烯烃的方法。该催化剂在700℃下单程C<sub>2+</sub>收率高达30.6%，且在甲烷分压高达1.4 atm的条件下仍能表现出稳定的性能。 </p> <div class="ueditorOption ueditorOptionModel" contenteditable="false" id="0" style="text-align: center;"> <img data-mce-="" data-wenge-id="66318" id="img-null" opaid="wenge-vkv7u1npmed0/" size="170890" src="https://rmtzx.sciencenet.cn//kxwsprint/65800649e4b03b5da6d05707.jpg" wosname="65800649e4b03b5da6d05707.jpg" /></div> <p class="timeLine_wg" style="height:20px;"> <span style="display:none"><span contenteditable="false" style="height: 0px; padding: 0px; margin: 0px; display: block; z-index: 9999; rgb(255, 255, 255); font-size: 0px; line-height: 0px; position: absolute; border-top: 1px dashed rgb(181, 189, 202); user-select: none; left: 0px; right: 0px; top: 8px;"><span class="timeIdentification" style="width:0px;height:0px;padding:0px;margin:0px;display:block;z-index:9999;#fff;position:absolute;font-size: 0px;line-height:0px;border-transparent;display:block;border-style:solid;right:0px;border-right-#B5BDCA;border-width:8px 8px 8px 0;top:-8px"> </span><span style="width:0px;height:0px;padding:0px;margin:0px;display:block;z-index:9999;#fff;position:absolute;font-size: 0px;line-height:0px;border-transparent;display:block;border-style:solid;left:0px;border-left-#B5BDCA;border-width:8px 0 8px 8px;top:-8px"> </span><span class="hide_time_wg" contenteditable="false" onclick="timeLine(this)" style="width:0px;height:0px;padding:0px;margin:0px;display:block;z-index:9999;#fff;position:absolute;font-size: 22px;line-height:17px;height:17px;text-align: center;width:17px;right:17px;background:#B5BDCA;cursor:pointer;top:-8px; border-radius: 2px;" title="在这插入段落">?</span></span></span></p> <p style=";; margin: 0px 0px 26px; text-align: center; word-break: break-all;"> 化学链甲烷氧化偶联反应机理解析。受访者供图</p> <p style=";; margin: 0px 0px 26px; text-align: justify; word-break: break-all;"> 甲烷氧化偶联（OCM）技术可在自热条件下通过一步反应将甲烷转化为高附加值烯烃或烷烃（C<sub>2+</sub>），是催化中的“圣杯反应”。但经过近40年的研究，常见的OCM催化剂Li/MgO和Na/Mn/W/SiO<sub>2</sub>等始终无法解决反应过程中C<sub>2+</sub>单程收率较低（<30%）、反应温度较高（>800°C）及甲烷反应气分压较低（<1 atm）等难题。</p> <p style=";; margin: 0px 0px 26px; text-align: justify; word-break: break-all;"> 该工作通过化学链循环的方式，构建了系列碳酸锂负载的复合稀土金属氧化物作为载氧体催化剂，有效抑制氧气直接作为氧化剂导致的甲烷过度氧化反应，进而实现甲烷氧化偶联高效制备C<sub>2+</sub>。通过原位表征手段与量子化学计算，发现复合稀土氧化物中的Pr<sup>4+</sup>可诱导催化剂表面产生过氧化物活性中间体并演变成活性羟基自由基，实现高效C-H键活化和C-C键偶联。 </p> <div class="ueditorOption ueditorOptionModel" contenteditable="false" id="1" style="text-align: center;"> <img data-mce-="" data-wenge-id="66320" id="img-null" opaid="wenge-m1txwlt72po0/" size="137528" src="https://rmtzx.sciencenet.cn//kxwsprint/65800670e4b03b5da6d0570b.png" wosname="65800670e4b03b5da6d0570b.png" /></div> <p class="timeLine_wg" style="height:20px;"> <span style="display:none"><span contenteditable="false" style="height: 0px; padding: 0px; margin: 0px; display: block; z-index: 9999; rgb(255, 255, 255); font-size: 0px; line-height: 0px; position: absolute; border-top: 1px dashed rgb(181, 189, 202); user-select: none; left: 0px; right: 0px; top: 8px;"><span class="timeIdentification" style="width:0px;height:0px;padding:0px;margin:0px;display:block;z-index:9999;#fff;position:absolute;font-size: 0px;line-height:0px;border-transparent;display:block;border-style:solid;right:0px;border-right-#B5BDCA;border-width:8px 8px 8px 0;top:-8px"> </span><span style="width:0px;height:0px;padding:0px;margin:0px;display:block;z-index:9999;#fff;position:absolute;font-size: 0px;line-height:0px;border-transparent;display:block;border-style:solid;left:0px;border-left-#B5BDCA;border-width:8px 0 8px 8px;top:-8px"> </span><span class="hide_time_wg" contenteditable="false" onclick="timeLine(this)" style="width:0px;height:0px;padding:0px;margin:0px;display:block;z-index:9999;#fff;position:absolute;font-size: 22px;line-height:17px;height:17px;text-align: center;width:17px;right:17px;background:#B5BDCA;cursor:pointer;top:-8px; border-radius: 2px;" title="在这插入段落">?</span></span></span></p> <p style=";; margin: 0px 0px 26px; text-align: center; word-break: break-all;"> 化学链甲烷氧化偶联反应性能。受访者供图</p> <p style=";; margin: 0px 0px 26px; text-align: justify; word-break: break-all;"> 该研究建立了Li<sub>2</sub>CO<sub>3</sub>负载的复合稀土金属氧化物中Pr的氧化态与C<sub>2+</sub>收率之间的普遍相关性，为甲烷氧化偶联反应中的氧化还原催化剂构建提供了理性设计思路。在此基础上，原料气还可以拓展至生物沼气、垃圾填埋气、煤层气等资源的高值化利用。</p> <div class="ueditorOption ueditorOptionModel" contenteditable="false" id="2" style="text-align: center;"> <img data-mce-="" data-wenge-id="66328" id="img-null" opaid="wenge-27brmjfojwg0/" size="17448" src="https://rmtzx.sciencenet.cn//kxwsprint/65800a5fe4b03b5da6d05717.jpg" wosname="65800a5fe4b03b5da6d05717.jpg" /></div> <p class="timeLine_wg" style="height:20px;"> <span style="display:none"><span contenteditable="false" style="height: 0px; padding: 0px; margin: 0px; display: block; z-index: 9999; rgb(255, 255, 255); font-size: 0px; line-height: 0px; position: absolute; border-top: 1px dashed rgb(181, 189, 202); user-select: none; left: 0px; right: 0px; top: 8px;"><span class="timeIdentification" style="width:0px;height:0px;padding:0px;margin:0px;display:block;z-index:9999;#fff;position:absolute;font-size: 0px;line-height:0px;border-transparent;display:block;border-style:solid;right:0px;border-right-#B5BDCA;border-width:8px 8px 8px 0;top:-8px"> </span><span style="width:0px;height:0px;padding:0px;margin:0px;display:block;z-index:9999;#fff;position:absolute;font-size: 0px;line-height:0px;border-transparent;display:block;border-style:solid;left:0px;border-left-#B5BDCA;border-width:8px 0 8px 8px;top:-8px"> </span><span class="hide_time_wg" contenteditable="false" onclick="timeLine(this)" style="width:0px;height:0px;padding:0px;margin:0px;display:block;z-index:9999;#fff;position:absolute;font-size: 22px;line-height:17px;height:17px;text-align: center;width:17px;right:17px;background:#B5BDCA;cursor:pointer;top:-8px; border-radius: 2px;" title="在这插入段落">?</span></span></span></p> <p style=";; margin: 0px 0px 26px; 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