Solubility and thermodynamics of lithium carbonate in sodium carbonate solution

doi:10.11949/0438-1157.20190647

Abstract

Abstract:

The isothermal dissolution equilibrium method was used to study the dissolution equilibrium of lithium carbonate in sodium carbonate solution (278.15—358.15 K), the lithium carbonate solubility and density were determined, and the experimental data of lithium carbonate solubility was correlated by E-DH equation, standard deviation of calculated is less than 0.1. The Connaughton equation is used to correlate the solution density data with a standard deviation of less than 2×10^-3. The experimental and theoretical results show that the solubility of lithium carbonate decreases first and then extremely slow decreases with the increase of sodium carbonate concentration in the temperature range of 278.15—358.15 K. Under the synergistic effect of the same ion effect and salt effect, the solubility change point is at sodium carbonate concentration of about 0.1 mol·kg^-1. The dissolution enthalpy (ΔH_d), entropy (ΔS_d) and Gibbs free energy (ΔG_d) of lithium carbonate in aqueous sodium carbonate solution were obtained by dissolution thermodynamic calculation. The results show that the dissolution process is a non-spontaneous process of exotherm and entropy reduction. The dissolution enthalpy and entropy increase with increasing sodium carbonate concentration, Gibbs free energy shows a maximum at 0.6 mol·kg^-1, and the dissolution process is an entropy controlled process. The research results will provide basic data for the design of lithium carbide precipitation process for brine.

Key words: lithium carbonate, sodium carbonate, solubility, E-DH equation, thermodynamic calculation

摘要：

采用等温溶解平衡法开展碳酸锂在碳酸钠溶液中(278.15～358.15 K)的溶解平衡实验研究，测定平衡体系碳酸锂溶解度和平衡溶液密度，利用E-DH方程对碳酸锂溶解度实验数据进行关联，标准偏差小于0.01；利用Connaughton方程对液相密度数据进行关联，标准偏差小于2×10^-3。实验和计算研究结果表明：在同离子和盐效应协同影响下，碳酸锂在Na₂CO₃-H₂O体系中溶解度随碳酸钠浓度增加先降低后降低趋势变缓，在278.15～358.15 K温度范围内，溶解度转变折点为碳酸钠浓度约为0.1 mol·kg^-1；通过溶解热力学计算，得到碳酸锂在碳酸钠中的溶解焓变(ΔH_d)、熵变(ΔS_d)和Gibbs自由能变(ΔG_d)，结果表明溶解过程为放热、熵减的非自发过程，溶解焓变和熵变随着碳酸钠浓度增加而增加，Gibbs自由能变在0.6 mol·kg^-1出现最大值，且溶解过程为熵控制过程。研究结果将为卤水提锂碳化沉锂过程设计提供基础数据。

关键词: 碳酸锂, 碳酸钠, 溶解度, E-DH方程, 热力学计算

CLC Number:

O 645.12

Haiwen GE, Huaiyou WANG, Min WANG. Solubility and thermodynamics of lithium carbonate in sodium carbonate solution[J]. CIESC Journal, 2019, 70(11): 4123-4130.

戈海文, 王怀有, 王敏. 碳酸锂在碳酸钠溶液中的溶解度与热力学[J]. 化工学报, 2019, 70(11): 4123-4130.

Figures/Tables 8

Table 1 Solubility and density of lithium carbonate in sodium carbonate solution at 278.15—358.15 K

$m N a 2 C O 3$ /

(mol·kg^-1)

$m L i 2 C O 3$ /

(mol·kg^-1)

ρ/(g·cm^-3)

$m N a 2 C O 3$ /

(mol·kg^-1)

$m L i 2 C O 3$ /

(mol·kg^-1)

ρ/(g·cm^-3)

$m N a 2 C O 3$ /

(mol·kg^-1)

$m L i 2 C O 3$ /

(mol·kg^-1)

0.0100

0.0203

0.0500

0.0699

0.1000

0.2869

0.4789

0.6521

0.8244

0.9938

1.1473

1.2808

1.4041

1.5801

1.6970

0.2122

0.2092

0.2066

0.2026

0.2007

0.1978

0.1887

0.1832

0.1795

0.1758

0.1723

0.1703

0.1689

0.1679

0.1667

0.1661

1.01319

1.01423

1.01502

1.01771

1.01939

1.02206

1.04224

1.05625

1.07596

1.09412

1.11250

1.12993

1.14522

1.16051

1.18297

1.19884

0.0100

0.0203

0.0500

0.0699

0.1000

0.2999

0.4697

0.6662

0.7975

0.9915

1.1504

1.2664

1.3503

1.4389

1.6734

0.1460

0.1448

0.1436

0.1416

0.1393

0.1377

0.1310

0.1287

0.1262

0.1251

0.1231

0.1217

0.1205

0.1198

0.1189

0.1167

1.00924

1.00981

1.01067

1.01260

1.01392

1.01614

1.03623

1.05277

1.07093

1.08600

1.10502

1.12462

1.13800

1.14748

1.15598

1.18412

0.0137

0.0225

0.0539

0.0691

0.0994

0.2808

0.3860

0.6659

0.8582

0.9944

1.0856

1.3309

1.4766

1.5863

1.7003

0.1118

0.1112

0.1102

0.1090

0.1076

0.1056

0.1036

0.1015

0.0998

0.0982

0.0974

0.0969

0.0965

0.0962

0.0959

0.0956

1.01021

1.01122

1.01190

1.01493

1.01629

1.01865

1.03587

1.04674

1.07783

1.09537

1.11162

1.12096

1.14863

1.16713

1.18202

1.19403

288.15 K

318.15 K

348.15 K

0.0100

0.0203

0.0500

0.0699

0.1000

0.2928

0.4807

0.6544

0.8328

0.9784

1.1560

1.2875

1.4490

1.5967

1.6958

0.1844

0.1826

0.1819

0.1799

0.1786

0.1766

0.1696

0.1652

0.1621

0.1595

0.1578

0.1558

0.1544

0.1528

0.1511

0.1502

0.99972

1.00068

1.00105

1.00411

1.00636

1.00809

1.02755

1.04397

1.06560

1.08103

1.09713

1.11942

1.13652

1.15176

1.16646

1.18660

0.0100

0.0203

0.0500

0.0699

0.1000

0.2999

0.4653

0.6580

0.7968

0.9975

1.1458

1.2717

1.3928

1.4461

1.6589

0.1313

0.1306

0.1293

0.1266

0.1252

0.1232

0.1204

0.1166

0.1145

0.1124

0.1111

0.1102

0.1098

0.1088

0.1084

0.1076

1.01180

1.01233

1.01326

1.01559

1.01740

1.01982

1.03942

1.05491

1.07592

1.09010

1.11190

1.12842

1.14393

1.15889

1.16700

1.19354

0.0122

0.0208

0.0549

0.0737

0.1022

0.2971

0.4153

0.6759

0.8569

1.0001

1.1851

1.3570

1.4941

1.6229

1.7651

0.1047

0.1036

0.1026

0.1012

0.1003

0.0981

0.0956

0.0924

0.0906

0.0890

0.0881

0.0873

0.0866

0.0861

0.0855

0.0849

1.01272

1.01350

1.01428

1.01740

1.01935

1.02091

1.03921

1.04953

1.07591

1.09373

1.10803

1.12868

1.14703

1.16309

1.17915

1.19600

298.15 K

328.15 K

358.15 K

0.0100

0.0203

0.0500

0.0699

0.1000

0.2999

0.4835

0.6689

0.8290

0.9987

1.1482

1.2904

1.4423

1.5847

1.7555

0.1643

0.1633

0.1618

0.1583

0.1560

0.1547

0.1484

0.1442

0.1408

0.1385

0.1361

0.1338

0.1327

0.1320

0.1312

0.1303

1.00455

1.00675

1.00740

1.00981

1.01393

1.01569

1.03510

1.05051

1.06890

1.08956

1.10256

1.12147

1.13787

1.15559

1.17257

1.19856

0.0159

0.0256

0.0511

0.0717

0.0975

0.2889

0.4551

0.6409

0.8074

0.9797

1.1256

1.2576

1.3728

1.5014

1.6558

0.1194

0.1184

0.1167

0.1157

0.1149

0.1126

0.1086

0.1071

0.1057

0.1047

0.1039

0.1033

0.1027

0.1025

0.1020

0.1016

1.01822

1.01927

1.02022

1.02325

1.02596

1.02867

1.05062

1.06883

1.08990

1.10916

1.13009

1.14910

1.16623

1.18240

1.20047

1.22193

0.0109

0.0199

0.0560

0.0723

0.1036

0.2932

0.4840

0.6559

0.8366

0.9871

1.1468

1.3385

1.4540

1.5811

1.7287

0.09532

0.09475

0.09337

0.09149

0.08955

0.08733

0.08459

0.08210

0.08052

0.07954

0.07892

0.07847

0.07802

0.07761

0.07730

0.07701

1.01048

1.01080

1.01143

1.01460

1.01586

1.01869

1.03549

1.05297

1.07208

1.08993

1.10670

1.12165

1.14762

1.15965

1.17548

1.19353

Table 1 Solubility and density of lithium carbonate in sodium carbonate solution at 278.15—358.15 K

$m N a 2 C O 3$ /

(mol·kg^-1)

$m L i 2 C O 3$ /

(mol·kg^-1)

ρ/(g·cm^-3)

$m N a 2 C O 3$ /

(mol·kg^-1)

$m L i 2 C O 3$ /

(mol·kg^-1)

ρ/(g·cm^-3)

$m N a 2 C O 3$ /

(mol·kg^-1)

$m L i 2 C O 3$ /

(mol·kg^-1)

ρ/(g·cm^-3)

278.15 K

308.15 K

338.15 K

0.0100

0.0203

0.0500

0.0699

0.1000

0.2869

0.4789

0.6521

0.8244

0.9938

1.1473

1.2808

1.4041

1.5801

1.6970

0.2122

0.2092

0.2066

0.2026

0.2007

0.1978

0.1887

0.1832

0.1795

0.1758

0.1723

0.1703

0.1689

0.1679

0.1667

0.1661

1.01319

1.01423

1.01502

1.01771

1.01939

1.02206

1.04224

1.05625

1.07596

1.09412

1.11250

1.12993

1.14522

1.16051

1.18297

1.19884

0.0100

0.0203

0.0500

0.0699

0.1000

0.2999

0.4697

0.6662

0.7975

0.9915

1.1504

1.2664

1.3503

1.4389

1.6734

0.1460

0.1448

0.1436

0.1416

0.1393

0.1377

0.1310

0.1287

0.1262

0.1251

0.1231

0.1217

0.1205

0.1198

0.1189

0.1167

1.00924

1.00981

1.01067

1.01260

1.01392

1.01614

1.03623

1.05277

1.07093

1.08600

1.10502

1.12462

1.13800

1.14748

1.15598

1.18412

0.0137

0.0225

0.0539

0.0691

0.0994

0.2808

0.3860

0.6659

0.8582

0.9944

1.0856

1.3309

1.4766

1.5863

1.7003

0.1118

0.1112

0.1102

0.1090

0.1076

0.1056

0.1036

0.1015

0.0998

0.0982

0.0974

0.0969

0.0965

0.0962

0.0959

0.0956

1.01021

1.01122

1.01190

1.01493

1.01629

1.01865

1.03587

1.04674

1.07783

1.09537

1.11162

1.12096

1.14863

1.16713

1.18202

1.19403

288.15 K

318.15 K

348.15 K

0.0100

0.0203

0.0500

0.0699

0.1000

0.2928

0.4807

0.6544

0.8328

0.9784

1.1560

1.2875

1.4490

1.5967

1.6958

0.1844

0.1826

0.1819

0.1799

0.1786

0.1766

0.1696

0.1652

0.1621

0.1595

0.1578

0.1558

0.1544

0.1528

0.1511

0.1502

0.99972

1.00068

1.00105

1.00411

1.00636

1.00809

1.02755

1.04397

1.06560

1.08103

1.09713

1.11942

1.13652

1.15176

1.16646

1.18660

0.0100

0.0203

0.0500

0.0699

0.1000

0.2999

0.4653

0.6580

0.7968

0.9975

1.1458

1.2717

1.3928

1.4461

1.6589

0.1313

0.1306

0.1293

0.1266

0.1252

0.1232

0.1204

0.1166

0.1145

0.1124

0.1111

0.1102

0.1098

0.1088

0.1084

0.1076

1.01180

1.01233

1.01326

1.01559

1.01740

1.01982

1.03942

1.05491

1.07592

1.09010

1.11190

1.12842

1.14393

1.15889

1.16700

1.19354

0.0122

0.0208

0.0549

0.0737

0.1022

0.2971

0.4153

0.6759

0.8569

1.0001

1.1851

1.3570

1.4941

1.6229

1.7651

0.1047

0.1036

0.1026

0.1012

0.1003

0.0981

0.0956

0.0924

0.0906

0.0890

0.0881

0.0873

0.0866

0.0861

0.0855

0.0849

1.01272

1.01350

1.01428

1.01740

1.01935

1.02091

1.03921

1.04953

1.07591

1.09373

1.10803

1.12868

1.14703

1.16309

1.17915

1.19600

298.15 K

328.15 K

358.15 K

0.0100

0.0203

0.0500

0.0699

0.1000

0.2999

0.4835

0.6689

0.8290

0.9987

1.1482

1.2904

1.4423

1.5847

1.7555

0.1643

0.1633

0.1618

0.1583

0.1560

0.1547

0.1484

0.1442

0.1408

0.1385

0.1361

0.1338

0.1327

0.1320

0.1312

0.1303

1.00455

1.00675

1.00740

1.00981

1.01393

1.01569

1.03510

1.05051

1.06890

1.08956

1.10256

1.12147

1.13787

1.15559

1.17257

1.19856

0.0159

0.0256

0.0511

0.0717

0.0975

0.2889

0.4551

0.6409

0.8074

0.9797

1.1256

1.2576

1.3728

1.5014

1.6558

0.1194

0.1184

0.1167

0.1157

0.1149

0.1126

0.1086

0.1071

0.1057

0.1047

0.1039

0.1033

0.1027

0.1025

0.1020

0.1016

1.01822

1.01927

1.02022

1.02325

1.02596

1.02867

1.05062

1.06883

1.08990

1.10916

1.13009

1.14910

1.16623

1.18240

1.20047

1.22193

0.0109

0.0199

0.0560

0.0723

0.1036

0.2932

0.4840

0.6559

0.8366

0.9871

1.1468

1.3385

1.4540

1.5811

1.7287

0.09532

0.09475

0.09337

0.09149

0.08955

0.08733

0.08459

0.08210

0.08052

0.07954

0.07892

0.07847

0.07802

0.07761

0.07730

0.07701

1.01048

1.01080

1.01143

1.01460

1.01586

1.01869

1.03549

1.05297

1.07208

1.08993

1.10670

1.12165

1.14762

1.15965

1.17548

1.19353

Fig.1 Solubility of lithium carbonate in sodium carbonate solution at different temperatures

Table 2 Model parameters and standard deviation of extended Debye-Hückel model at different temperatures

T/K

278.15

288.15

298.15

308.15

318.15

328.15

338.15

348.15

358.15

0.56776

0.52846

0.51160

0.48690

0.46413

0.44307

0.42357

0.40545

0.38859

24.19

25.66

28.58

28.32

30.95

35.60

42.61

50.17

54.66

-0.3154

-0.3636

-0.3621

-0.4050

-0.4273

-0.4465

-0.4499

-0.4438

-0.4551

0.02800

0.03444

0.03407

0.04128

0.04422

0.04593

0.04560

0.04510

0.04678

0.008213

0.009855

0.009934

0.008765

0.009765

0.009440

0.01059

0.01061

0.009062

Fig.2 Relative deviation of calculated concentration of Li+ experimental data for system Li2CO3-Na2CO3-H2O

Fig.3 Plot of dissolution enthalpy (ΔHd) of Li2CO3 against Na2CO3 molalities

Fig.4 Plot of dissolution entropy (ΔSd) of Li2CO3 against Na2CO3 molalities

Fig.5 Plot of dissolution Gibbs free energy (ΔSd) of Li2CO3 against Na2CO3 molalities

Table 3 Model parameters and standard deviation of Connaughton equation at different temperatures

T/K

a₁

b₁

a₂

b₂

278.15

288.15

298.15

308.15

318.15

328.15

338.15

348.15

358.15

0.7326

0.3796

1.558

0.1412

0.7893

2.095

0.8836

1.597

1.529

-1.461

-0.8787

-3.729

-0.1025

-1.730

-5.298

-1.852

-3.823

-3.545

0.05298

0.06969

0.03699

0.08134

0.06800

0.07174

0.08070

0.06645

0.06883

0.03858

0.02718

0.04579

0.01922

0.03088

0.03559

0.02107

0.02659

0.0281

0.9615×10^-3

1.894×10^-3

1.479×10^-3

0.7667×10^-3

0.6910×10^-3

0.5967×10^-3

0.8899×10^-3

0.5291×10^-3

0.8378×10^-3

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