Preparation of nano Cu-Mo2C interface supported on ordered mesoporous biochar of ultrahigh surface area for reverse water gas shift reaction

Biochar Pub Date : 2024-10-23 DOI:10.1007/s42773-024-00392-5
Xueyuan Pan, Hao Sun, Mingzhe Ma, Haiquan Liao, Guowu Zhan, Kui Wang, Mengmeng Fan, Jingcheng Xu, Linfei Ding, Kang Sun, Jianchun Jiang
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引用次数: 10

Abstract

Abstract High conversion rate and selectivity are challenges for CO 2 utilization through catalytic reverse water gas shift (RWGS) reaction. Herein, a novel mesoporous biochar (MB) supported Cu-Mo 2 C nano-interface was prepared by consecutive physical activation of coconut shells followed by carbothermal hydrogen reduction of bimetal. As compared with traditional carbon materials, this MB exhibited ultra-high specific surface area (2693 m 2 g –1 ) and mesopore volume of mesopore (0.81 cm 3 g –1 ) with a narrow distribution (2–5 nm), responsible for the high dispersion of binary Cu-Mo 2 C sites, CO 2 adsorption and mass transfer in the reaction system. Moderate carbothermal reduction led to the sufficient reduction of Mo ion with carbon matrix of MB and dispersive growth of nano Cu-Mo 2 C binary sites (~ 6.1 nm) on the surface of MB. Cu + species were formed from Cu 0 via electron transfer and showed high dispersion with simultaneous boosted bimetal loading due to the strong interaction between nano Mo 2 C and Cu. These were advantageous to the intrinsic activity and stability of the Cu-Mo 2 C binary sites and their accessibility to the reactant molecules. Under the RWGS reaction conditions of 500 °C, atmospheric pressure, and 300,000 ml/g/h gas hour space velocity, the CO 2 conversion rate over Cu-Mo 2 C/MB reached 27.74 × 10 –5 mol CO2 /g cat /s at very low H 2 partial pressure, which was more than twice that over traditional carbon supported Cu-Mo 2 C catalysts. In addition, this catalyst exhibited 99.08% CO selectivity and high stability for more than 50 h without a decrease in activity and selectivity. This study offers a new development strategy and a promising candidate for industrial RWGS. Graphical Abstract
超高表面积有序介孔生物炭负载纳米Cu-Mo2C界面的制备及反水气转换反应
摘要高转化率和高选择性是催化反水气转换(RWGS)反应利用co2面临的挑战。本文通过对椰壳进行连续物理活化,然后对双金属进行碳热氢还原,制备了一种新型介孔生物炭(MB)负载的Cu-Mo - C纳米界面。与传统的碳材料相比,该MB具有超高的比表面积(2693 m 2 g -1)和介孔体积(0.81 cm 3 g -1),且介孔分布窄(2 - 5 nm),是Cu-Mo 2 C二元位高度分散、CO 2吸附和传质的主要原因。适度的碳热还原导致Mo离子在MB的碳基体上充分还原,纳米Cu-Mo - C二元位(~ 6.1 nm)在MB表面分散生长。Cu +物质通过电子转移由Cu 0形成,由于纳米Mo - C与Cu之间的强相互作用,在双金属负载同时增强的情况下表现出高度分散。这有利于cu - mo2c二元位的固有活性和稳定性以及它们对反应物分子的接近性。在500℃、常压、30万ml/g/h气时空速的RWGS反应条件下,极低h2分压下Cu-Mo 2 C/MB的CO2转化率达到27.74 × 10 -5 mol CO2 /g cat /s,是传统碳负载Cu-Mo 2 C催化剂的2倍以上。该催化剂具有99.08%的CO选择性和50 h以上的高稳定性,且活性和选择性不降低。本研究为工业废水处理系统提供了新的发展策略和有前景的候选材料。图形抽象
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