Recent Progress on Electrocatalytic Synthesis of Ammonia Under Amibent Conditions

doi:10.6023/A20090412

Acta Chimica Sinica ›› 2021, Vol. 79 ›› Issue (2): 146-157.DOI: 10.6023/A20090412 Previous Articles Next Articles

Review

常温常压电催化合成氨的研究进展

詹溯¹, 章福祥¹^,^*()

1 中国科学院大连化学物理研究所大连 116023

投稿日期:2020-09-07 发布日期:2020-12-01
通讯作者: 章福祥

作者简介:

詹溯, 2017年于大连海事大学载运工具运用工程专业获得工学博士学位, 2018年加入中国科学院大连化学物理研究所章福祥课题组, 目前主要研究方向为常温常压光电催化合成氨.

章福祥, 中国科学院大连化物所研究员/博导; 国家杰出青年基金获得者; 英国皇家化学会会士. 1999和2004年分别获得南开大学理学学士学位和博士学位, 同年留校任教至2007年8月, 2007年9月至2008年6月获法国CNRS博士后基金支持于巴黎第六大学做访问学者, 2008年7月至2011年9月在东京大学做博士后和特任助理教授, 2011年10月至今在中国科学院大连化学物理研究所工作. 目前主要从事宽光谱捕光催化剂全分解水制氢研究, 研究内容涉及宽光谱捕光光催化材料设计合成, 高效光生电荷分离体系构建以及光催化表面/界面反应机制等方面. 已在包括Nat. Commun., Nature Catal., Joule, J. Am. Chem. Soc., Angew. Chem. Int. Ed., Adv. Mater., Adv. Energy Mater.等刊物上发表学术论文百余篇.

* E-mail: fxzhang@dicp.ac.cn

基金资助:
国家自然科学基金(21633009); 国家自然科学基金(21925206); 国家自然科学基金(21902159)

Recent Progress on Electrocatalytic Synthesis of Ammonia Under Amibent Conditions

Su Zhan¹, Fuxiang Zhang¹^,^*()

1 Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

Received:2020-09-07 Published:2020-12-01
Contact: Fuxiang Zhang
Supported by:
National Natural Science Foundation of China(21633009); National Natural Science Foundation of China(21925206); National Natural Science Foundation of China(21902159)

Ammonia is not only an important chemical for fertilizer and industrial chemical, but also an ideal carrier of clean energy. Current ammonia synthesis is mainly based on Haber-Bosch process that suffers from some problems such as high energy consumption, low conversion and large amount of greenhouse gas emission, so the solar ammonia synthesis from N₂ and H₂O has recently attracted extensive attention. However, both conversion and Faradaic efficiency via the solar-based catalysis have been still retarded by poor surface catalysis process. Accordingly, development of efficient electrocatalysts for N₂ reduciton reaction (NRR) as well as their coupling with photoadsorbers is highly desirable. The recent research progress in the following areas is summarized in this review: i) main electrocatalysts for NRR, including thermal catalyst, transition metal catalyst, noble metal catalyst and non-noble metal catalyst, ii) typical strategies to improve the NRR performance and iii) other routes using different nitrogen sources such as NO₃ ^– and NO. Finally, the remaining challenges and perspectives will be outlined.

Key words: ammonia synthesis, electrocatalysis, reduction of nitrogen, solar energy conversion, NO3– reduction, NO reduction

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Su Zhan, Fuxiang Zhang. Recent Progress on Electrocatalytic Synthesis of Ammonia Under Amibent Conditions[J]. Acta Chimica Sinica, 2021, 79(2): 146-157.

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反应式		电位/V (vs. NHE), pH=0
N₂+e^–→N₂ ^–	–4.16
N₂+H⁺+e^–→N₂H	–3.20
N₂+2H⁺+2e^–→N₂H₂	–1.10
N₂+4H⁺+4e^–→N₂H₄	–0.36
N₂+5H⁺+5e^–→N₂H₅ ⁺	–0.23
N₂+8H⁺+6e^–→2NH₄ ⁺	0.27
N₂+6H⁺+6e^–→NH₃	0.55

反应式		电位/V (vs. NHE), pH=0
N₂+e^–→N₂ ^–	–4.16
N₂+H⁺+e^–→N₂H	–3.20
N₂+2H⁺+2e^–→N₂H₂	–1.10
N₂+4H⁺+4e^–→N₂H₄	–0.36
N₂+5H⁺+5e^–→N₂H₅ ⁺	–0.23
N₂+8H⁺+6e^–→2NH₄ ⁺	0.27
N₂+6H⁺+6e^–→NH₃	0.55

检测方法	检测范围	特点	注意事项
纳氏试剂显色法	0.025~5.0 mg/L	操作简便	试剂中含汞, 毒性高, 对环境危害大, 试剂寿命短, 需要注意Fe²⁺、Cu²⁺、Ca²⁺等离子对显色效果干扰
水杨酸-次氯酸显色法	0.01~1.0 mg/L	操作简便、低毒性	溶液pH应大于11, 否则将影响显色化合物生成, 需要注意Fe²⁺离子对显色效果干扰
离子色谱	0.02~40 mg/L	重现性好、灵敏度高、检测时间短	注意电解液中Na⁺浓度, 减少对NH₄ ⁺检测的干扰
¹⁵N同位素-核磁共振NMR	5~10 μmol/L	为生成氨的真实来源提供直接证据	需保证¹⁵N₂气体的纯度

检测方法	检测范围	特点	注意事项
纳氏试剂显色法	0.025~5.0 mg/L	操作简便	试剂中含汞, 毒性高, 对环境危害大, 试剂寿命短, 需要注意Fe²⁺、Cu²⁺、Ca²⁺等离子对显色效果干扰
水杨酸-次氯酸显色法	0.01~1.0 mg/L	操作简便、低毒性	溶液pH应大于11, 否则将影响显色化合物生成, 需要注意Fe²⁺离子对显色效果干扰
离子色谱	0.02~40 mg/L	重现性好、灵敏度高、检测时间短	注意电解液中Na⁺浓度, 减少对NH₄ ⁺检测的干扰
¹⁵N同位素-核磁共振NMR	5~10 μmol/L	为生成氨的真实来源提供直接证据	需保证¹⁵N₂气体的纯度

	催化剂	电解液	NH₃产率	法拉第效率/%	文献
传统热催化剂	Fe₂O₃/CNT	KHCO₃	2.18×10^–3 g_NH3•m^–2•h^–1 (–2.0 V vs. Ag/AgCl)	0.025	[31]
	Fe-(O-C₂)₄	0.1 mol/L KOH	32.1 μg•h ^–1•mg_cat.^–1 (–0.1 V vs. RHE)	29.3	[33]
	Fe-N₄-C	0.1 mol/L KOH	7.48 μg•h ^–1•mg^–1 (0.0 V vs. RHE)	56.55	[34]
	Fe-W₁₈O₄₉	0.25 mol/L LiClO₄	24.7 μg•h ^–1•mg_cat. ^–1 (–0.15 V vs. RHE)	20.0	[65]
	Ru-Mo₂CT_x	0.5 mol/L K₂SO₄	40.57 μg•h ^–1•mg^–1 (–0.3 V vs. RHE)	25.77	[38]
	RuSAs/N-C	0.05 mol/L H₂SO₄	120.9 μg _NH3•mg_cat. ^–1•h^–1 (–0.3 V vs. RHE)	29.6	[39]
生物固氮酶同组分催化剂(Mo、V)	MoS₂	0.1 mol/L Na₂SO₄	8.08×10^–11 mol•s^–1•cm^–2 (–0.3 V vs. RHE)	1.17	[59]
	Mo₂N	0.1 mol/L HCl	78.4 μg•h ^–1•mg_cat. ^–1 (–0.3 V vs. RHE)	4.5	[60]
	SA-Mo/NPC	0.1 mol/L KOH	34.0 μg•h ^–1•g_cat. ^–1 (–0.3 V vs. RHE)	14.6	[43]
	Mo₃Fe₃C	0.1 mol/L Li₂SO₄	72.5 μg•h ^–1•cm^–2 (–0.05 V vs. RHE)	43.6	[69]
	V₈C₇	0.1 mol/L HCl	34.62 μg•h ^–1•cm^–2 (–0.4 V vs. RHE)	12.20	[45]
	VN	0.1 mol/L HCl	2.48×10^-10 mol^–1•s^–1•cm^–2 (–0.3 V vs. RHE)	3.58	[46]
	VO₂	0.1 mol/L Na₂SO₄	14.85 μg•h ^–1•g_cat. ^–1 (–0.7 V vs. RHE)	3.97	[61]
	P-V₂O₃/C	0.1 mol/L Na₂SO₄	22.4 μg•h ^–1•mg_cat. ^–1 (–0.35 V vs. RHE)	13.78	[62]
贵金属催化剂	Au纳米棒	0.1 mol/L KOH	1.648 μg•h ^–1•cm^–2 (–0.2 V vs. RHE)	4.02	[50]
	Au	0.1 mol/L HCl	21.4 μgh ^–1•mg_cat. ^–1 (–0.2 V vs. RHE)	8.11	[23]
	单原子Au	5 mmol/L H₂SO₄	1305 μg•h ^–1•mg_Au ^–1 (–0.1 V vs. RHE)	11.1	[51]
	单原子Pt	0.1 mol/L K₂SO₄	342.4 μg•h ^–1•mg_Pt ^–1 (–0.2 V vs. RHE)	31.3	[53]
	PdCu	0.1 mol/L KOH	2.8 μg•h ^–1•mg_cat. ^–1 (–0.2 V vs. RHE)	0.6	[48]
非贵金属催化剂	Cu-TiO₂	0.5 mol/L LiClO₄	21.31 μg•h ^–1•mg_cat. ^–1 (–0.55 V vs. RHE)	21.99	[54a]
	Sn枝晶	0.1 mol/L PBS	5.66×10^–11 mol^–1•s^–1•cm^–2 (–0.6 V vs. RHE)	3.67	[54b]
	Cr₂O₃/rGO	0.1 mol/L HCl	33.3 μg•h ^–1•mg_cat. ^–1 (–0.7 V vs. RHE)	7.33	[54c]
	LiMn₂O₄	0.1 mol/L HCl	15.83 μg•h ^–1•mg_cat. ^–1 (–0.5 V vs. RHE)	7.44	[54d]
	LaFeO₃	0.1 mol/L HCl	18.59 μg•h ^–1•mg_cat. ^–1 (–0.55 V vs. RHE)	8.77	[54e]
	Bi纳米片	0.1 mol/L HCl	6.89×10^–11 mol^–1•s^–1•cm^–2 (–0.5 V vs. RHE)	10.26	[56]

常温常压电催化合成氨的研究进展

Recent Progress on Electrocatalytic Synthesis of Ammonia Under Amibent Conditions

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