​四单位联合ACS Catal.: Ru单原子调节WO2酸性，促进碱性HER反应

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由可再生能源(如水、风和太阳能)驱动的水电解是一种有前景和有效的绿色氢气生产技术。在通用pH电解质中，碱性水电解一直被认为是工业制氢最可行的途径之一。然而，由于阴极析氢反应(HER)在高pH值介质中动力学缓慢，即使使用贵金属HER催化剂，碱性/中性HER活性比也比在酸中低2-3个数量级。


最近，有人在中性pH电解质中研究了一种由氧化钨载体和负载的贵金属(Ru和Ir)纳米颗粒组成的新型复合催化剂，其中弱酸性HxWO3中间体的形成改变了贵金属周围的酸性化学环境，从而显著提高了贵金属Ru/Ir的HER活性。然而，高价氧化钨的溶解问题限制了其在高pH条件下的进一步应用。因此，开发合理的策略来提高氧化钨的结构稳健性可能会显著促进贵金属催化剂的碱性HER过程。
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近日，中国科学院苏州纳米所崔义、苏州大学王璐、中国科学院上海高等研究院王娟和重庆理工大学陈志刚等通过水热法在泡沫镍表面制备了自支撑式WO2负载Ru单原子催化剂(Ru SAC@WO2/NF)。实验结果表明，在碱性介质中，所制备的Ru SAC@WO2/NF催化剂在10 mA cm−2电流密度下的HER过电位几乎为零，Tafel斜率为38 mV dec−1。
同时，该材料具有显著的实际应用价值，在电流密度为50和200 mA cm−2的条件下，过电位分别仅为40和84 mV，在100 mV过电位下的转换频率(TOF)为21.9 s−1。此外，Ru SAC@WO2/NF复合催化剂在10、50和200 mA cm−2条件下连续制氢50小时以上未发生明显地活性降解，显示出优异的反应稳定性。
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一系列表征结果和理论研究表明，Ru SAC@WO2/NF复合催化剂由于其固体酸催化剂的特性，可以改变碱性HER过程的传统反应途径：1.配位不饱和W原子作为高效的Lewis酸中心可自发或低能垒条件下产生质子；2.所产生的质子可以自发地插入WO2的晶格中以形成HxWOy弱酸中间体，这构建了酸性催化剂表面(pH<7)，并且Ru单原子中心通过遵循Volmer-Tafel反应途径加速相邻HxWOy位点的去质子化动力学以重新结合成H2分子。
此外，W-Ru金属键能够增强局部金属性质，将产生的OH−中间体排斥到碱性电解质中，进而保证了Ru单原子的稳定性。综上，该项研究通过结合具有酸性和金属性的WO2及Ru单原子的催化性能，为设计类酸性催化剂表面以强化高电流密度碱性HER反应提供了一条有价值的途径。
Ru single atoms tailoring the acidity of metallic tungsten dioxide for a boosted alkaline hydrogen evolution reaction. ACS Catalysis, 2024. DOI: 10.1021/acscatal.4c01173



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