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Cu Nanocluster-Loaded TiO2 Nanosheets for Highly Efficient Generation of CO-Free Hydrogen by Selective Photocatalytic Dehydrogenation of Methanol to Formaldehyde
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-04-13 , DOI: 10.1021/acsami.0c20116 Fengyang Yu 1 , Liyong Chen 1 , Xuezhao Li 1 , Xiaoshuang Shen 2 , He Zhao 3 , Chunying Duan 1 , Qianwang Chen 4
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-04-13 , DOI: 10.1021/acsami.0c20116 Fengyang Yu 1 , Liyong Chen 1 , Xuezhao Li 1 , Xiaoshuang Shen 2 , He Zhao 3 , Chunying Duan 1 , Qianwang Chen 4
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Safe storage and transportation of H2 is a fundamental requirement for its wide applications in the future. Controllable release of high-purity H2 from a stable storage medium such as CH3OH before use offers an efficient way of achieving this purpose. In our case, Cu nanoclusters uniformly dispersed onto (001) surfaces of TiO2 nanosheets (TiO2/Cu) are selectively prepared by thermal treatment of HKUST-1 loaded TiO2 nanosheets. One of the TiO2/Cu composites, TiO2/Cu_50, exhibits remarkably high activity toward the selective dehydrogenation of CH3OH to HCHO with a H2 evolution rate of 17.8 mmol h–1 per gram of catalyst within a 16-h photocatalytic reaction (quantum efficiency at 365 nm: 16.4%). Theoretical calculations reveal that interactions of Cu nanoclusters with TiO2 could affect their electronic structures, leading to higher adsorption energy of CH3OH at Ti sites and a lower barrier for the dehydrogenation of CH3OH by the synergistic effect of Cu nanoclusters and TiO2, and lower Gibbs free energy for desorption HCHO and H2 as well.
中文翻译：
Cu纳米团簇负载的TiO 2纳米片，用于通过甲醇的选择性光催化脱氢制甲醛来高效产生无CO氢。
H 2的安全储存和运输是未来其广泛应用的基本要求。使用前从稳定的存储介质（例如CH 3 OH）中可控地释放高纯度H 2提供了实现此目的的有效方法。在我们的情况下，通过热处理负载HKUST-1的TiO 2纳米片选择性地制备均匀分散在TiO 2纳米片（TiO 2 / Cu）的（001）表面上的Cu纳米簇。TiO 2 / Cu复合材料之一TiO 2 / Cu_50对CH 3 OH与H 2选择性脱氢为HCHO表现出显着的高活性。在16小时的光催化反应中，每克催化剂的析出速率为17.8 mmol h –1（365 nm处的量子效率：16.4％）。理论计算表明，Cu纳米团簇与TiO 2的相互作用会影响其电子结构，导致CH 3 OH在Ti位点的吸附能更高，并且由于Cu纳米团簇与TiO 2的协同作用而降低了CH 3 OH脱氢的势垒。，并且降低了吉布斯自由能，也使HCHO和H 2解吸。
更新日期：2021-04-29
中文翻译：
Cu纳米团簇负载的TiO 2纳米片，用于通过甲醇的选择性光催化脱氢制甲醛来高效产生无CO氢。
H 2的安全储存和运输是未来其广泛应用的基本要求。使用前从稳定的存储介质（例如CH 3 OH）中可控地释放高纯度H 2提供了实现此目的的有效方法。在我们的情况下，通过热处理负载HKUST-1的TiO 2纳米片选择性地制备均匀分散在TiO 2纳米片（TiO 2 / Cu）的（001）表面上的Cu纳米簇。TiO 2 / Cu复合材料之一TiO 2 / Cu_50对CH 3 OH与H 2选择性脱氢为HCHO表现出显着的高活性。在16小时的光催化反应中，每克催化剂的析出速率为17.8 mmol h –1（365 nm处的量子效率：16.4％）。理论计算表明，Cu纳米团簇与TiO 2的相互作用会影响其电子结构，导致CH 3 OH在Ti位点的吸附能更高，并且由于Cu纳米团簇与TiO 2的协同作用而降低了CH 3 OH脱氢的势垒。，并且降低了吉布斯自由能，也使HCHO和H 2解吸。
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