Construction of Ni-Based N-Doped Mesoporous Carbon Sphere for Efficiently Catalytic Dichromate Reduction with HCOOH at Room Temperature
Construction of Ni-Based N-Doped Mesoporous Carbon Sphere for Efficiently Catalytic Dichromate Reduction with HCOOH at Room Temperature
复制标题
室温下 HCOOH 高效催化重铬酸盐还原的镍基氮掺杂介孔碳球的构建
DOI：
10.1016/j.seppur.2022.121289
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发表时间：
2022-08
影响因子：
8.6
通讯作者：
Xiangke Wang
中科院分区：
文献类型：
--
作者：
Zhimin Lv;Shuya Liu;Yuxin Liu;Peisheng Liu;Ming Fang;Xiaoli Tan;Wei Xu;Mingguang Kong;Xiangke Wang
· Ni NPs@ N掺杂的碳球通过用Ni盐热解前体来制备，并用作还原Cr（VI）的催化剂。· Ni-N-C600可在7 min内完全还原高浓度Cr（VI）（100 mg/L，100 ml）。· Ni-N-C600对还原Cr（VI）显示出优异的上级活性、选择性和稳定性。·还原机理包括活性氢和官能团的电子贡献。有毒的Cr（VI）污染严重威胁着人们的健康，将Cr（VI）还原为Cr（III）已成为废水治理的一种高效途径。本文通过碳球与Ni盐的简单热解方法制备了金属Ni受限于N掺杂的介孔碳球的催化剂，并对用HCOOH还原Cr（VI）表现出显著的活性、选择性和稳定性。Ni-N-C600催化剂在室温下用HCOOH对高浓度Cr（VI）（100 mg/L，100 ml）的还原反应在7 min内即可达到100%的还原效果。即使存在共存离子（0.1 M Na +、K +、Ca 2+、Zn 2+、NO 3 −、Cl −、CO 3 2−和SO 4 2−），其催化效率也不会受到任何影响。Ni-N-C600的催化活性在循环5次后仍有很小的下降，这是由于介孔碳球物理屏障的限制作用阻止了Ni纳米颗粒的浸出和聚集。金属Ni的磁性极大地促进了催化剂的分离。还原机理主要是通过HCOOH脱氢产生的活性氢来实现的。此外，含碳官能团的电子供体也引起Cr（VI）的部分还原.本工作为设计和开发高效非贵金属催化剂还原Cr（VI）提供了理论依据。
• Ni NPs@N-doped carbon spheres are prepared by pyrolyzing precursors with Ni salts and utilized as a catalyst for reducing Cr(VI). • Ni-N-C600 can completely reduce the high concentrations of Cr(VI) (100 mg/L, 100 ml) within 7 min. • Ni-N-C600 shows superior activity, selectivity, and stability for reducing Cr(VI). • The reduction mechanism includes active hydrogen and electronic donation of functional groups. The pollution of poisonous Cr(VI) poses a severe threat to our health, and the reduction of Cr(VI) to Cr(III) has become a high-efficiency way for wastewater remediation. Herein, the catalyst with metallic Ni confined in an N-doped mesoporous carbon sphere was prepared by the easy pyrolysis method of carbon sphere with Ni salts and showed remarkable activity, selectivity, and stability for reducing Cr(VI) with HCOOH. Notably, the Ni-N-C600 can rapid and 100 % reduction of the high concentrations of Cr(VI) (100 mg/L, 100 ml) using HCOOH within 7 min at room temperature over the reported Ni-based catalysts. Even in the presence of coexisting ions (0.1 M of Na + , K + , Ca 2+ , Zn 2+ , NO 3 − , Cl − , CO 3 2− , and SO 4 2− ), its catalytic efficiency is not affected at all. The catalytic activity of the Ni-N-C600 declined little even after five cycles because the confinement effect of the mesoporous carbon sphere physical barrier prevented the leaching and aggregation of Ni NPs. The magnetism of metallic Ni greatly facilitates the separation of the catalyst. The reduction mechanism is mainly achieved by active hydrogen produced through the dehydrogenation of HCOOH. In addition, the electronic donation of C-containing functional groups also caused a partial reduction of Cr(VI). This work provides a rational design and development of high-efficiency non-noble metal catalysts to reduce Cr(VI).
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