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Conversion of CO2 to chemical feedstocks over bismuth nanosheets in situ grown on nitrogen-doped carbon
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2020-09-02 , DOI: 10.1039/d0ta07411j
Xin Wang 1, 2, 3, 4 , Wen-Jin Yin 4, 5, 6, 7 , Yubing Si 1, 2, 3, 4 , Xiaoming Wang 1, 2, 3, 4 , Xiaoxiao Guo 1, 2, 3, 4 , Wei Guo 1, 2, 3, 4 , Yongzhu Fu 1, 2, 3, 4
Affiliation  

The conversion of CO2 to value-added chemicals represents an attractive approach for CO2 utilization. Formate and methanol are sustainably valuable fuels and chemical feedstocks. However, the CO2 reduction reaction (CO2RR) suffers from unsatisfactory activity, low faradaic efficiency (FE) and inadequate durability. In this study, ultrathin bismuth nanosheets (NSs) and Bi NSs grown on nitrogen-doped ordered mesoporous carbon (OMC-N) are prepared from in situ transformation of atomic-thick Bi2O2Se and Bi2O2Se/OMC-N. Bi NSs enable efficient formate production with a large current density (51 mA cm−2 at −1.0 VRHE) and excellent selectivity (FE ≈ 90%). Interestingly, Bi NSs/OMC-N catalyzes the conversion of CO2 to formate and methanol simultaneously with maximum FEformate (70%) and FEmethanol (67%), and long-term stability (35 h). The composition produces 9.15 and 8.00 μmol cm−2 h−1 for formate and methanol at −0.67 VRHE, respectively, and methyl formate could be further prepared from the above products. Moreover, the generated Bi NSs achieve 288 mA cm−2 at −0.61 VRHE within a flow cell. Theoretical studies reveal that the activity for methanol is rationalized as the outcome of abundant pyridinic-N sites that stabilize the *COOH intermediate. Our study unveils the potential of hierarchical Bi NSs/OMC-N for an efficient and stable CO2RR to produce chemical feedstocks.

中文翻译:

氮掺杂碳上原位生长的铋纳米片上的CO2转化为化学原料

CO 2向增值化学品的转化代表了一种有吸引力的CO 2利用方法。甲酸盐和甲醇是具有可持续价值的燃料和化学原料。但是,CO 2还原反应(CO 2 RR)的活性不理想,法拉第效率(FE)低,并且耐久性不足。在这项研究中,通过原位原子级Bi 2 O 2 Se和Bi 2 O 2 Se / OMC-的原位转变制备了氮掺杂有序介孔碳(OMC-N)上生长的超薄铋纳米片(NSs)和Bi NSs。N. Bi NS能够以大电流密度(51 mA cm)有效地生成甲酸盐在-1.0 V RHE时为-2)和出色的选择性(FE≈90%)。有趣的是,Bi NSs / OMC-N催化了CO 2转化为甲酸和甲醇,同时具有最大的FE甲酸(70%)和FE甲醇(67%)以及长期稳定性(35 h)。该组合物在-0.67V RHE下分别产生甲酸和甲醇的9.15和8.00μmolcm -2 h -1,并且可以由上述产物进一步制备甲酸甲酯。此外,在-0.61 V RHE时,生成的Bi NSs达到288 mA cm -2在流通池中。理论研究表明,甲醇的活性被合理化为稳定* COOH中间体的大量吡啶N位的结果。我们的研究揭示了分层Bi NSs / OMC-N对于高效稳定CO 2 RR生产化学原料的潜力。
更新日期:2020-10-06
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