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γ-氧化铝从受污染的水中选择性吸附过渡族金属,以生产用于高效硝酸盐还原的双金属催化剂。

γ-AlO selectively adsorbs transition group metals from contaminated waters to produce bi-metallic catalysts for efficient nitrate reduction.

作者信息

Kim Deokhwan, Lee Chung-Seop, Lee Byoung Guan, Park Jaehyeong, Kim Ki Chul, Choe Jong Kwon, Westerhoff Paul, Rho Hojung

机构信息

Department of Environment Research, Korea Institute of Civil Engineering and Building Technology, 283 Goyang-Daero, Ilsanseo-Gu, Goyang-Si, Gyeonggi-Do 10223, Republic of Korea; Department of Construction Environment Engineering, KICT School, University of Science & Technology, 217 Gajeong-ro, Yuseong-gu, Daejeon 34113, Republic of Korea.

Environmental R&D Center, Institute of Environmental Science & Technology, SK Innovation, 325 Expo‑ro Yuseong‑gu, Daejeon 305‑712, Republic of Korea.

出版信息

J Hazard Mater. 2025 Aug 5;493:138428. doi: 10.1016/j.jhazmat.2025.138428. Epub 2025 Apr 28.

Abstract

Metals present in industrial or mining wastewater are hazardous to human health and the environment, and their remediation is costly. In this study, we used γ-AlO to capture transition metals (e.g., Pd, Cu, Ni, and Co) from wastewater and used the spent adsorbent as catalysts for nitrate reduction. Based on a pH-dependent surface-mediated redox reaction mechanism, Pd and Cu ions are selectively adsorbed onto γ-AlO at ambient temperature without involving the use of chemical reductants, thus transforming these pollutants into active catalytic sites. We particularly focused on Pd/Cu bimetallic catalysts, finding that the Pd and Cu ion concentrations in contaminated water impacted both nitrate reduction efficiency and nitrogen selectivity. The best nitrate reduction occurred with 0.74 wt% Pd and 0.66 wt% Cu on γ-AlO, achieving high nitrate reactivity and ∼81 % selectivity for N formation over 10 cycles. Ni and Co, which have smaller redox potential differences than Pd and Cu, showed limited interference with Pd and Cu adsorption, allowing γ-AlO to form Pd-Cu bimetallic catalysts selectively in batch and column tests. Overall, metal-based catalysts can be fabricated under ambient conditions while remediating metal-contaminated wastewater, thereby producing functional products (e.g., hydrogenation catalysts), which is consistent with circular economy principles.

摘要

工业或采矿废水中存在的金属对人类健康和环境有害,并且其修复成本高昂。在本研究中,我们使用γ-AlO从废水中捕获过渡金属(例如钯、铜、镍和钴),并将用过的吸附剂用作硝酸盐还原的催化剂。基于pH依赖的表面介导氧化还原反应机制,钯和铜离子在环境温度下被选择性吸附到γ-AlO上,无需使用化学还原剂,从而将这些污染物转化为活性催化位点。我们特别关注钯/铜双金属催化剂,发现污染水中的钯和铜离子浓度会影响硝酸盐还原效率和氮选择性。在γ-AlO上,当钯含量为0.74 wt%、铜含量为0.66 wt%时,硝酸盐还原效果最佳,在10个循环中实现了高硝酸盐反应活性和约81%的氮生成选择性。镍和钴的氧化还原电位差比钯和铜小,对钯和铜的吸附干扰有限,使得γ-AlO在分批和柱式试验中能够选择性地形成钯-铜双金属催化剂。总体而言,金属基催化剂可以在环境条件下制备,同时修复金属污染的废水,从而生产功能性产品(例如加氢催化剂),这符合循环经济原则。

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