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Ultrathin Phosphate-Modulated Co Phthalocyanine/g-C3N4 Heterojunction Photocatalysts with Single Co-N4 (II) Sites for Efficient O2 Activation.
Advanced Science ( IF 15.1 ) Pub Date : 2020-06-25 , DOI: 10.1002/advs.202001543 Xiaoyu Chu 1, 2, 3 , Yang Qu 1 , Amir Zada 1, 4 , Linlu Bai 1, 2 , Zhijun Li 1 , Fan Yang 1 , Lina Zhao 1, 3 , Guiling Zhang 2 , Xiaojun Sun 2 , Zhao-Di Yang 2 , Liqiang Jing 1
Advanced Science ( IF 15.1 ) Pub Date : 2020-06-25 , DOI: 10.1002/advs.202001543 Xiaoyu Chu 1, 2, 3 , Yang Qu 1 , Amir Zada 1, 4 , Linlu Bai 1, 2 , Zhijun Li 1 , Fan Yang 1 , Lina Zhao 1, 3 , Guiling Zhang 2 , Xiaojun Sun 2 , Zhao-Di Yang 2 , Liqiang Jing 1
Affiliation
Realization of solar‐driven aerobic organic transformation under atmospheric pressure raises the great challenge for efficiently activating O2 by tailored photocatalysts. Guided by theoretical calculation, phosphate groups are used to induce the construction of ultrathin Co phthalocyanine/g‐C3N4 heterojunctions (CoPc/P‐CN, ≈4 nm) via strengthened H‐bonding interfacial connection, achieving an unprecedented 14‐time photoactivity improvement for UV–vis aerobic 2,4‐dichlorophenol degradation compared to bulk CN by promoted activation of O2. It is validated that more •O2− radicals are produced through the improved photoreduction of O2 by accelerated photoelectron transfer from CN to the ligand of CoPc and then to the abundant single Co–N4 (II) catalytic sites, as endowed by the matched dimension, intimate interface even at the molecular level, and high CoPc dispersion of resulted heterojunctions. Interestingly, CoPc/P‐CN also exhibits outstanding photoactivities in the aerobic oxidation of aromatic alcohols. This work showcases a feasible route to realize efficient photocatalytic O2 activation by exploiting the potential of ultrathin metal phthalocyanine (MPc) assemblies with abundant single‐atom sites. More importantly, a universal facile strategy of H‐bonding‐dominating construction of MPc‐involved heterojunctions is successfully established.
中文翻译:
超薄磷酸盐调制 Co 酞菁/g-C3N4 异质结光催化剂,具有单个 Co-N4 (II) 位点,可有效激活 O2。
在大气压下实现太阳能驱动的好氧有机转化对通过定制光催化剂有效激活O 2提出了巨大的挑战。在理论计算的指导下,利用磷酸基团通过强化氢键界面连接诱导超薄Co酞菁/g-C 3 N 4异质结(CoPc/P-CN,≈4 nm)的构建,实现了前所未有的14倍与本体 CN 相比,通过促进 O 2的活化,UV-vis 需氧 2,4-二氯苯酚降解的光活性得到改善。经验证,通过加速光电子从 CN 转移到 CoPc 配体,然后转移到丰富的单一 Co-N 4 (II) 催化位点,改善 O 2 的光还原,产生更多的• O 2 -自由基,这归因于匹配的尺寸、甚至在分子水平上的紧密界面以及所得异质结的高CoPc分散度。有趣的是,CoPc/P-CN在芳香醇的有氧氧化中也表现出出色的光活性。这项工作展示了一种通过利用具有丰富单原子位点的超薄金属酞菁(MPc)组件的潜力来实现高效光催化O 2活化的可行途径。更重要的是,成功建立了一种以氢键为主的 MPc 异质结构建的通用简便策略。
更新日期:2020-08-19
中文翻译:
超薄磷酸盐调制 Co 酞菁/g-C3N4 异质结光催化剂,具有单个 Co-N4 (II) 位点,可有效激活 O2。
在大气压下实现太阳能驱动的好氧有机转化对通过定制光催化剂有效激活O 2提出了巨大的挑战。在理论计算的指导下,利用磷酸基团通过强化氢键界面连接诱导超薄Co酞菁/g-C 3 N 4异质结(CoPc/P-CN,≈4 nm)的构建,实现了前所未有的14倍与本体 CN 相比,通过促进 O 2的活化,UV-vis 需氧 2,4-二氯苯酚降解的光活性得到改善。经验证,通过加速光电子从 CN 转移到 CoPc 配体,然后转移到丰富的单一 Co-N 4 (II) 催化位点,改善 O 2 的光还原,产生更多的• O 2 -自由基,这归因于匹配的尺寸、甚至在分子水平上的紧密界面以及所得异质结的高CoPc分散度。有趣的是,CoPc/P-CN在芳香醇的有氧氧化中也表现出出色的光活性。这项工作展示了一种通过利用具有丰富单原子位点的超薄金属酞菁(MPc)组件的潜力来实现高效光催化O 2活化的可行途径。更重要的是,成功建立了一种以氢键为主的 MPc 异质结构建的通用简便策略。